IAEA-TECDOC-1429

Worldwide marine radioactivity

studies (WOMARS)
Radionuclide levels in oceans and seas
Final report of a coordinated research project

January 2005
IAEA-TECDOC-1429

Worldwide marine radioactivity

studies (WOMARS)
Radionuclide levels in oceans and seas
Final report of a coordinated research project

January 2005
 The originating Section of this publication in the IAEA was:
Radiometrics Laboratory
International Atomic Energy Agency
Marine Environment Laboratory
B.P. 800
MC 98012 Monaco Cedex

WORLDWIDE MARINE RADIOACTIVITY STUDIES (WOMARS)

RADIONUCLIDE LEVELS IN OCEANS AND SEAS
IAEA, VIENNA, 2004
IAEA-TECDOC-1429
ISBN 92–0–114904–2
ISSN 1011–4289
© IAEA, 2005
Printed by the IAEA in Austria
January 2005
 FOREWORD

The International Atomic Energy Agency's Marine Environment Laboratory in Monaco

has completed a four year Coordinated Research Project (CRP) on Worldwide Marine
Radioactivity Studies (WOMARS). The primary objective of the CRP was to develop an
understanding of the present open ocean distribution of radionuclides in the water column and
sediment and thus predict the radiological impact to be addressed, as well as to encourage and
support marine radioactivity studies in Member States by methodological assistance and total
analytical quality management. The project was designed with the intention of reviewing and
contributing to scientific knowledge of the processes which affect radionuclide distributions
and the sources which have introduced radionuclides to the world ocean.

The specific objectives of the CRP were to: identify the major sources of anthropogenic
radionuclides in the world ocean; develop present knowledge of the distributions of key
radionuclides (90Sr, 137Cs and 239,240Pu) in water and sediment of the world ocean; and study
the development of radionuclide concentrations in water with time using good quality
historical data (e.g. from the GEOSECS programme of the mid-1970s and new data sets
collected recently).

Two research coordination meetings were held (IAEA-MEL Monaco, 1999; Woods
Hole Oceanographic Institution, Woods Hole, USA, 2000) during which the objectives of the
CRP, the organization, data compilation, evaluation and synthesis were discussed. The
presentations and discussions covered both the development of average radionuclide
concentrations in surface water and in water profiles over the last twenty years. A. Aarkrog of
Denmark chaired the Research Co-ordination Meetings. The Scientific Secretary was P. P.
Povinec.

The topics covered were: Atlantic and Indian Oceans and their marginal seas (Working
Group 1); Pacific Ocean and its marginal seas (Working Group 2); Marine Processes
(Working Group 3).

The success of the CRP was due to the active collaboration of the chief scientific
investigators and the participating institutions as well as numerous other marine institutions
which provided radionuclide data for storage and evaluation for the project in the framework
of the development of the IAEA's Global Marine Radioactivity Database (GLOMARD). The
IAEA would like to express its gratitude for the information provided and for the very fruitful
cooperation.

The IAEA officer responsible for this publication was P.P. Povinec of the IAEA Marine
Environment Laboratory, Monaco.
 EDITORIAL NOTE

The use of particular designations of countries or territories does not imply any judgement by the
publisher, the IAEA, as to the legal status of such countries or territories, of their authorities and
institutions or of the delimitation of their boundaries.
The mention of names of specific companies or products (whether or not indicated as registered) does
not imply any intention to infringe proprietary rights, nor should it be construed as an endorsement
or recommendation on the part of the IAEA.
 CONTENTS

SUMMARY ............................................................................................................................... 1

1. INTRODUCTION ............................................................................................................ 3

2. INPUT OF ANTHROPOGENIC RADIONUCLIDES INTO THE

WORLD OCEAN ............................................................................................................. 5
2.1. Nuclear weapons testing ..................................................................................... 5
2.2. Nuclear reprocessing .......................................................................................... 9
2.3. The Chernobyl accident ...................................................................................... 9
2.4. Other nuclear accidents .................................................................................... 13
2.5. Sea dumping ..................................................................................................... 13
2.6. Use of radioisotopes ......................................................................................... 14
2.7. Hypothetical and potential inputs ..................................................................... 14
2.8. River runoff ...................................................................................................... 14
2.9. Summary of inputs............................................................................................ 15

3. PROCESSES AFFECTING RADIONUCLIDE CONCENTRATIONS AND

INVENTORIES IN THE OCEANS ............................................................................... 16
3.1. Radionuclides as oceanographic tracers ........................................................... 16
3.2. Fate of conservative vs. particle-reactive radionuclides ................................... 19
3.3. Variations in activity ratios............................................................................... 20
3.4. Variations in inventory ..................................................................................... 20

4. PACIFIC OCEAN .......................................................................................................... 23

4.1. Overview .......................................................................................................... 23
4.2. Radionuclides in the Pacific Ocean .................................................................. 24
4.3. Distribution of radionuclides in surface water and sediment ........................... 29
4.3.1. Surface water ........................................................................................ 29
4.3.2. Sediment ............................................................................................... 30
4.4. Surface water radionuclide time series ............................................................. 36
4.5. Water column radionuclide time series ............................................................ 53
4.6. Radionuclide inventories .................................................................................. 64
4.6.1. Water inventories .................................................................................. 64
4.6.2. Sediment inventories............................................................................. 64
4.7. Radionuclides in the Far Eastern Seas .............................................................. 73
4.7.1. Sea of Japan .......................................................................................... 73
4.7.2. The Sea of Okhotsk............................................................................... 76
4.7.3. The Yellow and East China Seas .......................................................... 76
5. INDIAN AND SOUTHERN OCEANS ......................................................................... 82
5.1. Radionuclides in surface water......................................................................... 82
5.2. Surface water radionuclide time series ............................................................. 83
5.3. Radionuclides in the water column .................................................................. 84

6. ATLANTIC AND ARCTIC OCEANS .......................................................................... 97

6.1. Surface water radionuclide time series in the Atlantic Ocean.......................... 98
6.2. Water column radionuclide time series in the Atlantic Ocean ....................... 105
6.3. Inventories of 90Sr and 137Cs in the NE Atlantic ............................................ 105
6.4. Radionuclides in northern European seas....................................................... 106
6.4.1. The Irish Sea ....................................................................................... 124
6.4.2. The North Sea ..................................................................................... 124
6.4.3. The Baltic Sea..................................................................................... 125
6.4.4. The Arctic Seas ................................................................................... 125
6.5. Radionuclides in the Mediterranean Sea ........................................................ 128
6.5.1. Surface water radionuclide time series ............................................... 129
6.5.2. Recent data on 137Cs and 239,240Pu in the water column of the
Mediterranean Sea .............................................................................. 131
6.5.3. Water column radionuclide time series .............................................. 133
6.5.4. Radionuclide inventories in the water column of the
Mediterranean Sea .............................................................................. 133
6.5.5. Radionuclide inventories in the deep Mediterranean Sea................... 137

7. CONCLUSIONS .......................................................................................................... 137

REFERENCES....................................................................................................................... 145

ANNEX I. TRANSFER COEFFICIENTS FOR 90Sr AND 137Cs FOR

DOSE CALCULATIONS ................................................................................... 153

ANNEX II. LIST OF PUBLICATIONS PUBLISHED BY THE IAEA-MEL/RML STAFF

ON WORLDWIDE MARINE RADIOACTIVITY STUDIES ......................... 159

ANNEX III. 137Cs, 90Sr AND 239,240 Pu BIBLIOGRAPHY FOR THE

PACIFIC AND INDIAN OCEANS .................................................................. 163

CONTRIBUTORS TO DRAFTING AND REVIEW ........................................................... 187

 SUMMARY
This publication summarizes the results of the Coordinated Research Project (CRP) on
Worldwide Marine Radioactivity Studies (WOMARS) carried out by the IAEA's Marine
Environment Laboratory in Monaco. It provides the most comprehensive information on
levels of anthropogenic radionuclides in the world ocean. Three anthropogenic radionuclides
— 90Sr, 137Cs and 239,240Pu were chosen as the most representative of anthropogenic
radioactivity in the marine environment, comprising beta-, gamma- and alpha-emitters which
have the highest potential contribution to radiation doses to humans via seafood consumption.
Although the ocean contains the majority of the anthropogenic radionuclides released into the
environment, the radiological impact of this contamination is low. Radiation doses from
naturally-occurring radionuclides in the marine environment (e.g. 210Po) are on the average
two orders of magnitude higher.
The results confirm that the dominant source of anthropogenic radionuclides in the
marine environment is global fallout. The total 137Cs input from global fallout was estimated
to be 311 PBq for the Pacific Ocean, 201 PBq for the Atlantic Ocean, 84 PBq for the Indian
Ocean and 7.4 PBq for the Arctic Ocean. For comparison, 5 about 40 PBq of 137Cs was
released to the marine environment from Sellafield and Cap de la Hague reprocessing plants.
The Chernobyl accident contributed about 16 PBq of 137Cs to the sea, mainly the Baltic and
Black Seas, where the present average concentrations of 137Cs in surface water were estimated
to be about 60 and 25 Bq/m3, respectively, while the worldwide average concentration due to
global fallout is about 2 Bq/m3.
For the purposes of this study, the world ocean was divided into latitudinal belts for
which average radionuclide concentrations were estimated. Further, where available, time
trends in radionuclide concentrations in surface water were studied and mean residence times
of radionuclides in these areas as well as in the world ocean were estimated. The results
confirm similar mean residence times for 90Sr and 137Cs in surface water, 28 ± 3 years and
13 ± 1 year for 239,240Pu.
Changes in radionuclide concentrations in water profiles with time in the North Atlantic
and Pacific Oceans were also studied. A clear decrease of radionuclide concentrations in
surface water was observed due to transport of radionuclides to medium water depths.
The results obtained in the framework of the WOMARS CRP provide the most
complete data set available to Member States on levels of anthropogenic radionuclides in the
marine environment. The results will be used as the international reference source on the
average levels of anthropogenic radionuclides in the marine environment so that any further
contributions from nuclear reprocessing plants, radioactive waste disposal sites, nuclear bomb
test sites and possible nuclear accidents can be identified.

1
 1. INTRODUCTION

Radionuclides have been released to the environment from a multiplicity of sources,

both planned and accidental. Given that more than 70% of the surface of the Earth is ocean, it
is not surprising that much of these releases now reside there. The largest ocean, the Pacific,
has been a major repository for these releases — in part because of its sheer size, and in part
due to localized releases there.
There has been a growing number of known sources of anthropogenic radionuclides in
the marine environment. They include global nuclear fallout following atmospheric weapons
tests, the Chernobyl accident, discharges of radionuclides from nuclear installations, dumping
of nuclear wastes into the world's oceans and seas, nuclear submarine accidents, contributions
from nuclear weapons tests sites, loss of nuclear weapons and radioactive sources, and
satellite burnup.
Due to variations in the source inputs and subsequent dispersion, mixing and transport
of radionuclides in the world's oceans and seas, the marine environment is labelled with
radionuclides differing from one region to another according to the predominant source there.
The main global source of radionuclides in the marine environment is fallout from
nuclear tests performed in the atmosphere. In some regions, like the Irish, Baltic and Black
Seas, the concentration of 137Cs in the marine environment depends on the input due to
discharges from reprocessing facilities and from the Chernobyl accident, and in these regions
the evolution of its concentration is quite dynamic.

The interest in, and relevance of knowledge of the behaviour of radionuclides in the
ocean derives from a variety of issues. Firstly, the fate of radionuclides needs to be well
understood to provide the basis for an assessment of adverse environmental or human health
consequences, real or perceived. Then, this accumulated knowledge provides a critical basis
for rapid assessment of the impact of future releases — especially unplanned ones. These
include accidents involving radionuclide releases from such sources as coastal nuclear
facilities, nuclear waste disposal sites or from maritime transport of nuclear fuel or nuclear
wastes. Finally, radionuclides are powerful tracers providing basic insights into a variety of
oceanic processes. For example, plutonium as a particle active radio-element, is readily
incorporated into several compartments of the ocean carbon cycle. Because of the relatively
well defined temporal and spatial aspects of its introduction to the ocean, its movement within
the ocean provides many insights into a large number of processes in the oceanic water
column, and in biological and sedimentary systems.

Assessment of marine radioactivity in a given region therefore requires knowledge of

the source terms and an understanding of oceanic processes. The deposition of radionuclides
from these sources is unevenly distributed over the world ocean. The input function of global
fallout in the world ocean, mainly due to nuclear weapons tests carried out in the sixties, can
be estimated from worldwide monitoring mainly performed on land. On the other hand,
discharges from nuclear fuel reprocessing plants or dumping of liquid and solid radioactive
wastes have generally had a more local character, although soluble radionuclides have been
transported over long distances by prevailing currents.

In order to estimate radionuclide inputs from local sources, radionuclide distributions in

the world’s oceans and seas must be better known so that results from scientific expeditions to
nuclear waste dumping sites and/or other sources of anthropogenic marine radioactivity can
be reviewed objectively, comparatively and comprehensively. This requires a detailed study

3
of the present distributions and inventories of the main radionuclides of interest (3H, 14C, 90Sr,
137
Cs and Pu isotopes) in the world’s oceans and seas as well as possible predictions of their
concentrations in the near future.

As a contribution to these investigations, in 1995 the International Atomic Energy

Agency’s Marine Environment Laboratory (IAEA-MEL) commenced a seven year project
"Research on Worldwide Marine Radioactivity" with the generous support of the Science and
Technology Agency (STA) of the Government of Japan. As part of this project a four year
(1998–2001) Coordinated Research Project (CRP) entitled "Worldwide Marine Radioactivity
Studies (WOMARS)" was carried out.
The objectives of the CRP were to :
(i) Identify the major sources of anthropogenic radionuclides in the world ocean,
(ii) Develop present knowledge of the distributions of key radionuclides (90Sr, 137
Cs
and Pu isotopes) in water and sediment of the world ocean,
(iii) Study the development of radionuclide concentrations in water with time using
good quality historical data (e.g. from the GEOSECS programme of the mid-1970s
and new data sets collected recently).

The main aim of the CRP was to develop an understanding of the present open ocean
distribution of radionuclides in the water column and sediment and thus predict the
radiological impact to be addressed. Further, to encourage and support marine radioactivity
studies in Member States by methodological assistance and total analytical control
management. The project was designed to review and contribute to scientific knowledge of
the processes affecting radionuclide distributions and the sources which have introduced
radionuclides to the world ocean.

Three anthropogenic radionuclides (90Sr, 137Cs and 239,240Pu) were chosen as the most
important and radiologically typical for beta-, gamma- and alpha-emitters. They are the most
abundant anthropogenic radionuclides of each class present in the marine environment and
can lead to the highest radiation doses to humans and marine biota.

In this publication, the state of knowledge of the distribution and behaviour of

radionuclides in the world ocean and indications of the changes which have evolved over time
are discussed. It will not constitute a comprehensive review of all studies involving
radionuclides in the ocean but will try to cover the most relevant aspects. The studies cited
generally provide reference to a related work and thus fuller details should be sought in the
quite large literature base on this topic.

The CRP participants collected large amounts of data from their respective regions of
interest as well as from other regions, consideration being given to the entire coverage of the
oceans of the world. In addition, specific tasks were assigned to collect information from
countries not participating in the CRP so that these data could also be included in the Global
Marine Radioactivity Database (GLOMARD), which is under development in the
Radiometrics Laboratory at IAEA-MEL.
The information collected is of high scientific value and represents a reference source
on average radionuclide levels in the marine environment. The present report summarizes the
results obtained in the framework of the CRP.

4
 2. INPUT OF ANTHROPOGENIC RADIONUCLIDES INTO
THE WORLD OCEAN

The world ocean covers an area of 361.11·106 km2 or 70.8% of the total surface of the
Earth [1]. Hence, the ocean is a major recipient of anthropogenic radionuclides released to the
environment by atmospheric as well as aquatic pathways.

The oceans may receive radioactive fallout directly from the atmosphere and indirectly
as runoff from rivers. Radionuclides may, however, also be discharged directly into the ocean
as liquid waste or from dumped solid wastes. Some radionuclides will behave conservatively
and stay in the water in soluble form, whereas others will be insoluble or adhere to particles
and thus, sooner or later, be transferred to marine sediments.

The three main sources of anthropogenic radionuclides are nuclear weapons testing in
the atmosphere, the Chernobyl accident and water-borne discharges from nuclear reprocessing
plants, notably Sellafield in the UK and Cap de la Hague in France [2]. Other sources e.g. sea
dumping of nuclear waste, routine discharges from nuclear power plants, sunken nuclear
submarines, satellite losses, lost nuclear weapons and the use of radioisotopes in medicine,
industry and science, contribute orders of magnitude less to the contamination of the world
ocean than the three major sources.

The aim of this chapter is, on the basis of the most recent information [2] to present an
estimate of the input of anthropogenic radionuclides to the world ocean, and to calculate the
inventories of these radionuclides as of the year 2000. As 90Sr and in particular 137Cs are the
main contributors to the present radiation doses from man-made sources in the environment
[3], the focus is on these two radionuclides.

2.1. Nuclear weapons testing

Atmospheric nuclear test explosions have contaminated the Earth globally with
radioactive debris. The weapons tested from 1945 to 1951 were fission weapons in the 20–
100 kilotons TNT range. They produced mainly tropospheric fallout, i.e. the debris remained
below the tropopause and was not dispersed globally, but was deposited around the latitude
band of the test site. However, in 1952 the United States and in 1953 the former Soviet Union
(FSU) tested their first thermonuclear devices (megatons TNT range) and fallout from these
explosions occurred worldwide. In the following years and up until the early sixties the major
inputs of radionuclides from nuclear weapons testing occurred at Novaya Zemlya Island in the
Arctic Ocean (80.89 Mt fission yield) and at Bikini Atoll in the Pacific Ocean (42.2 Mt fission
yield). Other important locations in this respect have been Enewetak and Johnston Atolls in
the North Pacific (26 Mt), Christmas Island in the Indian Ocean (15.5 Mt), Lop Nor in China
(12.2 Mt), Mururoa and Fangataufa Atolls in the South Pacific (6.1 Mt) and Semipalatinsk in
Kazakhstan (3.7 Mt).

The distribution of global fallout (based on data from [2]) is shown in Fig. 1. The data
are from a worldwide network of land-based measuring stations for 90Sr in fallout. The global
fallout pattern first of all reflects the atmospheric transport of debris from the stratosphere to
the troposphere with maximum transfer at the mid-latitudes. The global precipitation pattern
and the locations of the test sites also influence the global distribution of weapons fallout. The
significantly lower amount of fallout in the Southern hemisphere is due to the relatively low
number of test explosions there, but also to the limited atmospheric exchange between the
northern and southern stratospheres.

5
 3.5

2.5

kBq/m²
2

1.5

0.5

0
90 80 70 60 50 40 30 20 10 0 10 20 30 40 50 60 70 80 90

Northern hemisphere Southern hemisphere

90
FIG. 1. Integrated deposition density of Sr (kBq/m2) (cumulative deposition is 0.40 x
integrated in 2000) [2].

Table I shows the inputs of 90Sr and 137Cs from global fallout to the various parts of the
world ocean based on fallout over land. The 137Cs data were obtained from 90Sr data by
multiplying by 1.6 [2]. The deposition densities (Bq/m2) in the various latitude bands were
from [2] and the ocean areas were obtained from [1]. Figure 2 shows the relative input of 90Sr
from global fallout to the various parts of the world ocean. The relative areas of the four
oceans compared to the total area of the world ocean are for the Pacific, Atlantic, Indian and
Arctic Oceans: 50%, 26%, 20% and 4%, respectively. Hence, the Indian and Arctic Oceans
have received less input of 90Sr from global fallout than could be expected from their
respective areas, whereas the Atlantic has received about 25% more than expected. The
discrepancies are explained by the lower fallout to the Arctic and Southern hemisphere than to
the temperate regions of the Northern hemisphere (see also Fig. 3 where the latitudinal
distribution of 90Sr input in PBq is shown). In this context it should be noted that present
radionuclide inventories in the Arctic Ocean are higher than those expected from direct input
due to transport from temperate latitudes in the North Atlantic via the Norwegian Coastal
Current.

In order to obtain the actual (year 2000) inventories in the world ocean, the values in
Table I should be decay-corrected by a factor of 0.40. The same decay factor has been used
for both 90Sr and 137Cs.

UNSCEAR [2] has, based on the fission yields of the nuclear weapons tested, reported
the global release (PBq) of those radionuclides which have been globally dispersed in
atmospheric nuclear testing. Table II shows those still present in the environment.

6
TABLE I. INPUTS FROM GLOBAL FALLOUT (PBq)

Summary of 90Sr input to the world ocean from global fallout

Latitude Arctic Atlantic Indian Pacific Total Ocean area 1012m2

Ocean Ocean Ocean Ocean
N 90º-60º 4.6 10.2 0.0 1.3 16.1 17.2
N 60º-30º 0.0 57.3 0.0 71.6 128.9 46.8
N 30º-0º 0.0 30.8 13.3 65.8 109.9 90.6
S 0º-30º 0.0 10.3 14.6 26.6 51.5 98.0
S 30º-60º 0.0 15.4 22.5 25.8 63.7 88.2
S 60º-90º 0.0 1.7 2.1 3 6.8 20.4
Total 4.6 125.7 52.5 194.1 376.9 361.1

Summary of 137Cs input to the world ocean from global fallout

N 90º-60º 7.4 16.3 0.0 2.1 25.8

N 60º-30º 0.0 91.7 0.0 114.6 206.2
N 30º-0º 0.0 49.3 21.3 105.3 175.8
S 0º-30º 0.0 16.5 23.4 42.6 82.4
S 30º-60º 0.0 24.6 36.0 41.3 101.9
S 60º-90º 0.0 2.7 3.4 4.8 10.9
Total 7.4 201.1 84.0 310.6 603.0

A rctic
1%

A tla n tic
33%

P a cific
52%

In d ia n
14%

FIG. 2. Relative input of 90Sr from global fallout to the world ocean.

The inputs to the ocean for 90Sr and 137Cs were taken from Table I. The other radionuclides
were calculated from 90Sr and their release ratios to 90Sr. As 241Pu decays to 241Am with a
half-life of 14.35 years, most of the 241Pu deposited in the ocean (and elsewhere) has already
decayed to 241Am.

7
 140

120

100

80
PBq
60

40

20

FIG. 3. Input of 90Sr from global fallout to the ocean.

0
N 90- N 60- N 30-0 S 0-30 S 30- S 60-

TABLE II. GLOBAL FALLOUT RADIONUCLIDES STILL PRESENT IN PBq-

QUANTITIES IN THE YEAR 2000
Nuclide Half-life Global Release Input Ocean
release ratio to to inventory
90
Sr ocean 2000
(year) (PBq) (PBq) (PBq)
3
H 12.33 186000 299 112693 13300
14
C 5730 213 0.3424 129 128
90
Sr 28.78 622 1 377 151
137
Cs 30.07 948 1.52 603 251
239
Pu 24110 6.52 0.0105 4.0 4.0
240
Pu 6563 4.35 0.007 2.6 2.6
241
Pu 14.35 142 0.2283 86 13.7

According to [2] the total fission yield of atmospheric nuclear test explosions is 189 Mt
(TNT). The production estimate of 90Sr is 3.88 PBq Mt-1. Hence, the total production of 90Sr
from nuclear weapons testing in the atmosphere is 733 PBq. However, 29 Mt (corresponding
to 113 PBq 90Sr) were not globally dispersed, but were deposited as local fallout close to the
test sites. Hence, only 160 Mt or 622 PBq 90Sr became global fallout. Since about 2–3% of
90
Sr decayed before deposition, the total amount deposited is calculated to be 605 PBq 90Sr.
From measurements of the global deposition of 90Sr (Fig. 1), the global input from nuclear
weapons testing in the atmosphere is calculated to be 604 PBq 90Sr. It may thus be concluded
that measurements and calculations from fission yields agree.

As nearly all local fallout (28 Mt fission) occurred at the US test sites at Bikini and
Enewetak Atolls in the Pacific Ocean (0–30˚N latitude belt), it is assumed that this part of the
Pacific Ocean may have received about 113 PBq 90Sr besides the 66 PBq 90Sr (see Table I)
received from global fallout. However, the 113 PBq may not be fully dispersed in sea water as
some of it is imbedded in minerals (corals). Hence, it is difficult to estimate to what extent the
inventory of 90Sr in the world ocean has increased from this source. It is even more difficult to

8
estimate the contribution from local fallout for the other radionuclides mentioned in Table II.
Only actual environmental measurements in this part of the Pacific Ocean can give an
indication of the possible contamination to the world ocean from local fallout at Bikini and
Enewetak.

Local fallout from the Novaya Zemlya test site has probably not contributed
significantly to the radionuclide inventories in the ocean. According to [2], the debris from
these tests went almost entirely (96%) to the stratosphere. Less than 0.5% was distributed as
local and regional fallout and the remaining part was deposited as tropospheric fallout.

2.2. Nuclear reprocessing

Reprocessing is carried out to recover U and Pu from spent fuel for reuse in reactors.
The major reprocessing plants are in the United Kingdom (Sellafield), France (Cap de La
Hague) and Japan (Tokai). Sellafield has been the major source of radioactive contamination
of the marine environment. In the 1970s British Nuclear Fuel Ltd., Sellafield (earlier
Windscale), began to substantially increase its authorized water-borne radioactive discharges
to the Irish Sea. These discharges, first of all of 137Cs, but also other radionuclides, notably
plutonium isotopes, americium and technetium, have become measurable in most parts of the
NE Atlantic and to a large extent in the Arctic Ocean. Table III and Figs 4 and 5 show the
annual liquid discharges of 137Cs and 90Sr from Sellafield and Cap de La Hague, respectively.
Furthermore, the decay-corrected amounts (to year 2000) are shown. While the 90Sr
discharges from Cap de la Hague amounted to 20% of those from Sellafield, the discharges of
137
Cs were less than 3% of the corresponding Sellafield releases. Apart from the 40 PBq 137Cs
and 6.5 PBq 90Sr released from the two European reprocessing plants, 126 PBq 3H, 1 PBq
99
Tc and 0.015 PBq 129I contribute to the contamination of the ocean at present and the NE
Atlantic (30-90°N) in particular. Whereas the input of 3H from reprocessing is negligible
compared with that from global fallout (see Table II), Sellafield and La Hague are major
sources to the oceanic inventories of 99Tc and 129I. These two very long lived radionuclides
(half-lives: 213,000 and 1,570,000 years, respectively) will remain in the marine environment
long after all the other radionuclides mentioned in this context (Table II) have disappeared.

2.3. The Chernobyl accident

Approximately two thirds of the ~100 PBq 137Cs released by the Chernobyl accident in
1986 were deposited outside the former Soviet Union [4]. Although most of this activity fell
over land, a significant part went to the sea. In particular, the European marginal seas received
a substantial amount of the Chernobyl debris. The Baltic Sea was the most contaminated. The
total inventory from the accident was calculated to be 4.5 PBq 137Cs [5]. Since Chernobyl, the
Baltic Sea has been a main source of fresh inflow of 137Cs to the NE Atlantic Ocean.
The Black Sea received 2–3 PBq 137Cs from the Chernobyl accident [6]. The outflow
from the Black Sea is the main source of “new” 137Cs in the Mediterranean Sea. However, the
inflow is less than the decay of the present 137Cs Chernobyl Mediterranean Sea inventory of
3–5 PBq. The Mediterranean Sea also received direct fallout from the accident. From German
and British measurements it has been estimated [7], that the North Sea received 1.2 PBq 137Cs
from Chernobyl. The Chernobyl inventory in the NE Atlantic was estimated at about 6 PBq
137
Cs. In the summer of 1987, surface sea water samples collected in the Greenland,
Norwegian and Barents Seas and off the west coast of Norway and the Faroe Islands, all
contained Chernobyl-derived 137Cs.

9
TABLE III. RADIOACTIVE DISCHARGES FROM SELLAFIELD AND CAP DE LA
HAGUE, 1970–1998 IN TBq

Sellafield Cap de la Hague

137 90 137 90 137 90 137 90
Year Cs Sr Cs ac Sr ac Cs Sr Cs ac Sr ac
1970 1200 230 600 112 89 2 45 1
1971 1300 460 665 229 243 8 124 4
1972 1289 562 675 286 33 16 17 8
1973 770 280 413 146 69 19 37 10
1974 4100 390 2249 208 56 52 31 28
1975 5230 466 2936 255 34 38 19 21
1976 4289 381 2464 214 35 20 20 11
1977 4480 427 2634 245 51 36 30 21
1978 4090 597 2460 351 39 70 23 41
1979 2600 250 1601 151 23 56 14 34
1980 2970 352 1871 217 27 29 17 18
1981 2360 277 1522 175 39 27 25 17
1982 2000 319 1320 207 51 86 34 56
1983 1200 204 810 135 23 142 16 94
1984 434 72 300 49 30 110 21 75
1985 325 52 230 36 29 47 21 33
1986 18 18 13 13 10 69 7 49
1987 12 15 9 11 8 57 6 42
1988 13 10 10 7 9 40 7 30
1989 29 9 22 7 13 29 10 22
1990 24 4 19 3 13 16 10 13
1991 15 4 12 3 6 30 5 24
1992 15 4 12 3 3 18 2 15
1993 22 17 19 14 4 25 3 21
1994 14 29 12 25 11 16 10 14
1995 12 28 11 25 5 30 4 27
1996 10 16 9 15 2 11 2 10
1997 8 37 7 34 3 4 3 4
1998 8 18 7 17 3 3 3 3
Total 38837 5528 22911 3195 961 1106 566 744

Note: ac is the actual activity by the year 2000.

The total Chernobyl 137Cs input to the world ocean is estimated at about 16 PBq. It has
been assumed here that the input of 90Sr to the sea was negligible. The inputs of 137Cs were
estimated at 10 PBq in the 30–60˚N latitude belt and at 6 PBq in the 60–90˚N belt. Nearly all
137
Cs went to the N Atlantic and Arctic Oceans. The relative input to the ocean thus became
significantly less than that from nuclear weapons fallout, because the Chernobyl accident was
a tropospheric event, first of all contaminating the surrounding European land areas.

10
 5500
Strontium 90
5000
Caesium 137
Radioactive discharges from Sellafield, 1986-1998 in TBq
4500
40
4000 35
30
3500 25
20
15
3000
10

Total Activity (TBq)

5
2500 0
1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998
2000 Years

Total Activity (TBq)

1500

1000

500

0
1970 1972 1974 1976 1978 1980 1982 1984 1986 1988 1990 1992 1994 1996 1998

FIG.4. Radioactive discharges from Sellafield, 1986-1998 in TBq.

11
12
260

240 Strontium 90
220 Caesium 137
200

180

160

140

120

100

Total Activity (TBq)

80

60

40

20

0
1970 1971 1972 1973 1974 1975 1976 1977 1978 1979 1980 1981 1982 1983 1984 1985 1986 1987 1988 1989 1990 1991 1992 1993 1994 1995 1996 1997 1998

Years

FIG. 5. Radioactive discharges from Cap de la Hague, 1970–1998 in TBq.

2.4. Other nuclear accidents

A few nuclear accidents have released radionuclides directly into the sea. Most
accidents have, however, involved releases to the atmosphere. The marine environment has
thus received only indirect contamination either from atmospheric deposition or through
runoff from land.

The two major nuclear accidents in 1957, Kyshtym and Windscale, are not believed to
have contributed significantly to the contamination of the marine environment.

In 1968 a US B-52 aircraft crashed during an emergency landing on sea-ice 11 km west

of Thule Airbase in NW Greenland. A similar accident had occurred two years previously at
Palomares in SE Spain [8], but the radioactive debris from that accident had mainly been
deposited on land. At Thule, the marine environment became contaminated with about 1 TBq
239,240
Pu [9].

A number of nuclear submarines, American as well as Russian, have been lost in the
world ocean. The most recent loss was the Russian submarine "Kursk" in the Barents Sea in
August 2000. This submarine was recovered in 2001 and no contamination of the sea
occurred. Another loss was the Soviet "Komsomolets" submarine, which sank at a depth of
1700 m at Bear Island in the eastern part of the Norwegian Sea. The activity in the wreck is
estimated at 2.8 PBq 90Sr and 3 PBq 137Cs, and the nuclear warheads may contain 16 TBq
239,240
Pu [10]. Close to the "Komsomolets", slightly enhanced levels of 137Cs have been
measured in sea water, but the sunken nuclear submarines may be considered only as potential
sources to radioactive contamination of the ocean.

Some satellites are nuclear powered. On a few occasions such satellites have burned up
in the upper atmosphere and have thereby contributed to the contamination of the ocean. This
was the case in 1964 when a SNAP-9A nuclear power generator aboard a US satellite re-
entered the atmosphere in the Southern hemisphere [11]. The generator contained 0.6 PBq
238
Pu. Since the accident, seawater samples from the Southern hemisphere have shown an
enhanced 238Pu/239,240Pu ratio, compared to ocean water from the Northern hemisphere.

2.5. Sea dumping

Sea dumping in the western world was carried out on a national basis, from the late
1940s to the mid-1960s, mainly by the US in the Atlantic and Pacific Oceans and by the UK
in the NE Atlantic. In 1967, the European Nuclear Energy Agency (later NEA) organized an
international operation where about 0.3 PBq solid waste was deposited at a depth of 5 km in
the eastern Atlantic Ocean. Similar international operations continued until 1982. At that time
about 0.7 PBq α activity, 42 PBq β activity and 15 PBq tritium had been dumped in the N
Atlantic [7, 12]. The Coordinated Research and Environmental Surveillance Programme
Related to Sea Disposal of Radioactive Waste "CRESP" has assessed the radiological impact
of the NEA dumping activities [13]. Minor releases of Pu from the dumped waste have been
measured at the dumpsite.

The former Soviet Union (FSU) disposed of radioactive waste for over three decades in
the Kara and Barents Seas. The total amount of waste dumped in the Arctic Seas was
estimated to be approximately 90 PBq [14]. The International Arctic Seas Assessment Project
(IASAP) study [15] has estimated that the inventory in 1993/94 had decayed to 4.7 PBq.
Monitoring has shown [10], that the releases from the dumping sites are small. Model
calculations have demonstrated that the total collective dose over the next 1000 years to the

13
world's population from the Russian dumpsite is in the order of 10 man Sv [15]. This is 300
times less than the corresponding dose from the radioactive waste dumped in the NE Atlantic
[13].

2.6. Use of radioisotopes

Radioisotopes are used in medicine, industry and research. Those most widely used as
unsealed sources are usually short lived, e.g. 99mTc and 131I and are thus of no importance as
sources to worldwide marine contamination. Hence, although the global usage of 131I in
nuclear therapy is approximately 0.6 PBq, it does not result in a measurable inventory in the
world ocean.

Longer lived radionuclides such as 3H and 14C are used in research, but releases to the
environment are very low and compared to the oceanic inventories from global fallout, of no
significance.

2.7. Hypothetical and potential inputs

During 1949–1951, medium and low level liquid radioactive waste from the Soviet
nuclear establishment, Mayak in the South Urals was released into the Techa River. In total
100 PBq were discharged. 90Sr and 137Cs contributed 11.6% and 12.2%, respectively [16].
Most of the activity was retained in a cascade of reservoirs in the upper reaches of the Techa
River, which is part of the Ob River system. Although the distance from Mayak to the outlet
of the Ob River in the Arctic Ocean is about 2000 km, it cannot be ruled out that 90Sr which is
more mobile than 137Cs, may have reached the Arctic Ocean around 1950. The contamination
may be estimated to be in the order of 1 PBq [17].

Since 1951, Lake Karachay at Mayak has been used for disposal of radioactive waste.
The lake has received 3.6 EBq 137Cs and 0.74 EBq 90Sr [18]. Lake Karachay is a potential
source for future contamination of the Ob River system and thus of the Arctic Ocean. The
Krasnoyarsk Mining and Chemical Complex is another hypothetical source to radioactive
contamination of the Arctic Ocean. Other nuclear installations in the FSU (and elsewhere)
should also be kept in mind in this context. In e.g. Murmansk and Vladivostok, radioactive
waste is stored in the military naval bases and at remote locations, also along the Siberian
coastline lighthouses are powered by 90Sr generators. Each generator contains in the order of
10 PBq 90Sr and in the event of an accident is a potential source of environmental
contamination. A 90Sr generator was lost in the Sea of Okhotsk, but no contamination has
been reported.

2.8. River runoff

Radionuclides deposited in the terrestrial environment may be transported to

groundwater, lakes and rivers, and later to the sea. Runoff is thus a secondary transfer of
atmospheric radioactivity to the sea. About 9% of the 90Sr inventory on land will be removed
by runoff [19]. For 137Cs the figure is about 2% [20].

As the total deposits of global fallout 90Sr and 137Cs are 622 PBq and 948 PBq,
respectively, and as 377 PBq 90Sr and 603 PBq 137Cs were deposited in the sea, the terrestrial
input has been 245 PBq 90Sr and 345 PBq 137Cs. Furthermore, the total deposition from
Chernobyl was ~10 PBq 90Sr and ~85 PBq 137Cs [2]. Of this, 10 PBq 90Sr and 69 PBq 137Cs
fell over land.

14
 The global runoff of 90Sr is thus calculated as: 0.09(245+10) 23 PBq and that of 137Cs
becomes: 0.02(345+69) = 8 PBq. By the year 2000 these inputs would have decayed to about
9 PBq 90Sr and 3 PBq 137Cs. In other words runoff may increase the 90Sr inventory in the
world ocean by 6% and the 137Cs inventory by 1–2%, which is insignificant when other
uncertainties are taken into consideration. Furthermore, radionuclides transported by runoff
will often be bound to particulates and thus be sedimented rather than transferred to biota.
Hence, runoff is not believed to influence the marine pathway ingestion doses to man
significantly.

2.9. Summary of inputs

The total input from all sources of 90Sr to the world ocean has been 383 PBq (377 PBq
from global fallout and 6.5 PBq from reprocessing). The input of 137Cs was 659 PBq (604
PBq from fallout, 40 PBq from reprocessing plants) and 16 PBq from Chernobyl. To these
figures should be added local inputs in the equatorial N Pacific, which may be in the order of
100 PBq for each of the two radionuclides. Table IV summarizes the present (year 2000)
inventories of 90Sr, 137Cs and 239,240Pu in the world ocean from all major sources, including
local fallout.
TABLE IV. RADIONUCLIDE INVENTORIES IN THE YEAR 2000 IN THE WORLD
OCEAN (PBq)

Arctic & Atlantic Oceans Indian & Pacific World

Oceans

Latitude Global Local Repro- Chernoby Subtotal Global Local Subtotal ALL
fallout fallout cessing l fallout fallout SOURCE
S
90
Sr
N 90º-30º 28.8 0.0 3.9 0.0 32.7 29.2 0.0 29.2 61.9
N 30º-0º 12.3 0.0 0.0 0.0 12.3 31.6 22.5 54.1 66.5
S 0º-30º 4.1 0.0 0.0 0.0 4.1 16.5 22.5 39.0 43.1
S 30º-90º 6.8 0.0 0.0 0.0 6.8 21.4 0.0 21.4 28.2
TOTAL 52.1 0.0 3.9 0.0 56.0 98.6 45.0 143.6 199.7
137
Cs
N 90º-30º 46.1 0.0 23.5 11.5 81.1 46.7 0.0 46.7 127.8
N 30º-0º 19.7 0.0 0.0 0.0 19.7 50.6 36.0 86.6 106.3
S 0º-30º 6.6 0.0 0.0 0.0 6.6 26.4 36.0 62.4 69.0
S 30º-90º 10.9 0.0 0.0 0.0 10.9 34.2 0.0 34.2 45.1
TOTAL 83.4 0.0 23.5 11.5 118.4 157.8 72.0 229.8 348.2
239,240
Pu
N 90º-30º 1.3 0.0 0.0 0.0 1.3 1.3 0.0 1.3 2.5
N 30º-0º 0.5 0.0 0.0 0.0 0.5 1.4 1.0 2.4 2.9
S 0º-30º 0.2 0.0 0.0 0.0 0.2 0.7 1.0 1.7 1.9
S 30º-90º 0.3 0.0 0.0 0.0 0.3 0.9 0.0 0.9 1.2
TOTAL 2.3 0.0 0.0 0.0 2.3 4.3 2.0 6.3 8.6
It has been assumed that the inputs of local fallout from the US Pacific tests were 113 PBq 90Sr, 181 PBq 137Cs
and 2 PBq 239,240Pu. It was further assumed that this fallout was equally divided between latitude bands N 30-0°
and S 0-30°. 90Sr and 137Cs had by the year 2000 decayed to 45 PBq and 72 PBq, respectively.

15
 The major inputs from global fallout occurred in the late fifties and early sixties,
reprocessing discharges peaked in the last half of the seventies and nearly all of the fallout
from Chernobyl was deposited in 1986. There has been some redistribution of the
radionuclides in the ocean due to both advection and mixing processes. Water-borne releases
from reprocessing in western Europe and global fallout have thus been dispersed to the Arctic
Ocean and contamination from the Baltic Sea, due to the Chernobyl accident, has reached the
North Atlantic and Arctic Oceans.
The NE Atlantic is the part of the world ocean most contaminated by radionuclides
because of 137Cs input from all three major sources: global fallout, reprocessing and
Chernobyl. The lowest input of anthropogenic radionuclides has been to the waters
surrounding the Antarctic continent. In these southern parts of the Pacific, Indian and Atlantic
Oceans, the concentrations of e.g. 137Cs are about 40 times lower than those found in the NE
Atlantic [21].
Although the ocean contains most of the anthropogenic radionuclides released into the
environment, the radiological impact of this contamination is low. Radiation doses from
naturally-occurring radionuclides in the marine environment (e.g. 210Po), are on the average
two orders of magnitude higher [21].

3. PROCESSES AFFECTING RADIONUCLIDE CONCENTRATIONS AND

INVENTORIES IN THE OCEANS

A wide range of radionuclides has been released into the oceans. Their distribution in
space and time can be quite complex, but is always related to four general processes: the input
function/source, radioactive decay, biogeochemistry, and oceanic processes.

A brief review of each of these processes is made below and provides examples and
references to studies that incorporate these processes into the interpretation of environmental
radionuclide distributions and inventories. It suffices to say that in most instances,
considerable ancillary, non-radiochemical data are needed to interpret ocean radionuclide
distributions. Thus the most basic studies require a knowledge of local oceanographic
conditions in addition to the physical properties of the radionuclide of interest. This review
will focus primarily on the man-made, or anthropogenic radionuclides, though considerable
effort has been spent in ocean sciences understanding naturally-occurring radionuclides, such
as the uranium/thorium decay series. Insights into the expected fate of anthropogenic
radionuclides can often be gained by comparisons between appropriate natural and
anthropogenic radionuclides.

3.1. Radionuclides as oceanographic tracers

The most fundamental properties needed to understand marine radionuclide

distributions are the half-life of the radionuclide, and information on its source. While those
isotopes with the shortest half-lives (<days - months) often are of greatest radioecological
concern (131I, t1/2 = 8.0 days), radionuclides with longer half-lives pose a greater potential for
redistribution, bioaccumulation, and storage within the oceans and underlying sediment. Also
useful with respect to half-lives, is the ability to identify different radionuclide sources, due to
the presence of shorter-lived isotopes in any particular sample. For example, the presence of
134
Cs (t1/2 = 2.07 yrs) in surface ocean water shortly after the Chernobyl accident, allowed for
the separation of Cs derived from the more recent 1986 source and prior sources of Cs such as
weapons testing fallout which by the 80s, had essentially zero 134Cs [22].

16
TABLE V. CHARACTERISTIC ISOTOPIC RATIOS COMMONLY USED TO IDENTIFY
ANTHROPOGENIC RADIONUCLIDE SOURCES IN THE MARINE ENVIRONMENT
240
Source Pu/239Pu atom ratio
Global weapons testing fallout 0.18
Nevada test site 0.03
Pacific test sites >0.30
Novaya Zemlya/Barents Sea <0.03
Mururoa <0.06
134
Source Cs/137Cs activity ratio in 1986
Global weapons testing fallout 0
Chernobyl fallout 0.5
137
Source Cs/90Sr activity ratio
Global weapons testing fallout 1.5 (in 1962, peak fallout year)
Chernobyl fallout 5 (in 1986, year of release)
Sellafield discharges 11 (in 1975, peak discharge
year)

If decay-corrected to April 26, 1986, 134Cs/137Cs ratios of 0.5 were found to be

characteristic of the source and subsequent fallout (Table V [23]). Similar examples of using
short lived radionuclides to pinpoint a source can be found from the early weapons testing
years (e.g. 141Ce and 144Ce in deep ocean sea cucumbers [24]).

All radionuclide data are reported with a reference date, generally either the sampling
date or date of release, so that changes in the reported distributions can be attributed to
environmental, rather than decay processes. Sources of anthropogenic radionuclides have
been reviewed elsewhere (this report, Chapter 2, [25, 26]).

Many of the anthropogenic radionuclides from both fallout and local sources have been
used by oceanographers as "tracers" of marine processes. Of great interest, for example in
ocean sciences, has been the distribution of fallout 14C and tritium as tracers of the rates of
ocean mixing (see below). It should also be noted in this regard that fallout delivery to the
Northern hemisphere was much greater than to the Southern hemisphere, thus for the world
ocean, there are generally lower activities of all anthropogenic radionuclides in sea water,
sediment and biota south of the equator. Also, due to local fallout from weapons tests
conducted in the Pacific, the inventories of Pu for example are higher than in soil samples at
comparable latitudes (Fig. 6). In terms of local sources, there has been considerable use of
Sellafield-derived 137Cs and 90Sr (Fig. 7), and Cap de la Hague-derived 129I to trace water
movement in the North and Baltic Seas and into the Arctic Ocean [27, 28]. An additional
category of local source input to the ocean is found in indirect input from rivers draining into
the ocean. An example of this would be delivery of 90Sr from the Chernobyl reactor site via
the Dnepr river to the Black Sea (Fig. 8 [29]).

17
FIG. 6. 239,240Pu inventories in Pacific water columns (mCi/km2) from GEOSECS [30]. Note
that the water column inventories in the NW Pacific are higher than those expected from
global fallout delivery (column on the right), due to local fallout from testing at Enewetak and
Bikini.

FIG. 7. Surface distributions of 137Cs (disintegrations per minute per 100 kg as of 1 January
1981) in the Norwegian-Greenland Seas. Samples were collected in 1981 (dark symbols) and
1982 (light symbols). Note highest values north of Scotland due to Sellafield discharges [27].

18
FIG. 8. Average 90Sr concentrations in the Dnepr river near the Black Sea. Total fluxes per
year are also indicated. Note large increase in 90Sr concentrations after Chernobyl [29].

3.2. Fate of conservative vs. particle-reactive radionuclides

Once released into the ocean, the fate of each isotope is largely tied to its chemical
properties. Broadly speaking, the anthropogenic radionuclides are divided into:

(i) conservative, or
(ii) non-conservative or so-called particle-reactive radionuclides.

Conservative tracers are defined as being highly soluble in sea water, thus their
redistribution upon entering the ocean is determined largely by physical processes related to
ocean mixing and diffusion. Common examples of conservative radionuclides include 137Cs,
90
Sr, 14C, tritium, 129I. Particle-reactive elements undergo more rapid removal from the ocean
due to the affinity of these elements for natural particle surfaces and the general rain of
sinking particles in the ocean which removes these particle-bound isotopes to the deep sea and
underlying sediment. Examples include 239,240Pu, 106Ru and 144Ce.

A cause of confusion in marine radionuclide studies is that, depending upon the local
ocean conditions and the time-scales of interest, different radionuclides can be used as both
conservative and non-conservative tracers. For example, Cs is commonly used as a
conservative tracer. However particle fluxes are considerably higher in coastal and more
productive waters than in the open ocean, hence, 137Cs can be more readily scavenged in the
coastal ocean and once bound to clays, can be used in sediment as a tracer of particle mixing
and sediment accumulation. While Pu is generally thought of as a non-conservative tracer, its
distribution on time-scales of years is largely controlled by physical mixing especially in the
open ocean. Contrasting chemical behaviour of reduced Pu (more particle-reactive) and
oxidized Pu (more soluble), leads to more rapid and complete removal of Pu from anoxic
waters such as the deep Black Sea [31], thus in this case local geochemistry leads to
conservative vs. non-conservative behaviour. Not only chemical, but also the physical form in
which a radionuclide is delivered may determine its fate. For example, it has been shown that
local fallout from land-based testing has delivered Pu to the oceans that was more rapidly
removed to deep ocean sediment than its stratospheric-based Pu counterpart. It was
hypothesized that this was due to the incorporation of Pu into melted silicate sands from the

19
 240
Nevada Test Site (Figs 9 & 10) [32]. In this case, the measurements of Pu/239Pu isotopic
ratios were used to identify the different Pu sources (Table V).

3.3. Variations in activity ratios

Since many anthropogenic radionuclides are introduced into the oceans in constant, or
known local ratios, the change in ratio with time or location can often be used to deduce the
extent and rates of particle reactivity for a given pair. For example, 239,240Pu/137Cs ratios in sea
water decreased rapidly, due to removal of Pu onto particles and subsequent vertical sinking
of these Pu-bearing particles (Fig. 11). Thus, by the time of the GEOSECS programmes in the
1970s, surface water Pu/Cs ratios in the central Pacific of <0.002 had been found, and in
vertical profiles of both radionuclides this ratio increased to >0.02. Pu was found throughout
all depths to 6000 m in at least low levels, while 137Cs was not detected in deep water [30].

Another way in which activity ratios might be observed to change is in a two

dimensional sense, with enhanced removal of particle-reactive tracers occurring at ocean
margins. Since surface mixing times between ocean gyres and margins is in the order of years
to decades, horizontal transport can bring two radionuclides from the central basin in fallout
proportions to ocean boundaries, but the more particle-reactive species would be enriched in
coastal sediment (and depleted in coastal water) due to enhanced scavenging. With time, there
would be a continued separation and removal of slightly particle-reactive species in ocean
margins, thus leading to an increase in time, for example, in the Pu/Cs ratio in coastal
sediment as Pu continues to be scavenged relative to Cs.

In addition to vertical and horizontal fractionation of conservative and non-conservative

elements in sea water, there is also the possibility of post-depositional mobility of one or
another species, depending upon geochemical conditions. One example, is the continued
release of Cs and Pu from the contaminated sediment at the Marshall Islands (Fig. 12). On the
other hand, it is known that in highly reducing marine sediments, pore water concentrations of
NH4 increase and under these conditions Cs becomes more mobile [33, 34] and thus more
diffusive. This is evidenced by Cs being found deeper in sediment than Pu delivered at the
same time, and its loss to overlying waters.

3.4. Variations in inventory

As might be expected from the discussion above, variations in total inventory (per
volume of water, sediment, or per area) are often important in order to learn more about the
behaviour of radionuclides in the oceans. Most useful in this regard is some knowledge of
delivery patterns (in space and time) and total supply per unit area of the ocean (assuming
fallout delivery). Soil samples provide particularly useful information for determining average
delivery rates, relative source ratios and inventories of many fallout radionuclides in each
latitudinal band [35]. Due to higher than expected Pu (and Cs, Sr) inventories in sea water and
sediment, it was possible to deduce, for example, that the N Pacific was impacted by local
fallout from US weapons testing at the Pacific Proving Grounds [30]. Inventories were also
used to examine the strength of boundary scavenging along the coast for 239,240Pu and
naturally-occurring excess 210Pb (Fig. 13) [36].

20
FIG. 9. 240Pu/239Pu atom ratios in sediments vs. depth in the NW Atlantic. Squares were
sampled in 1983-1985, while diamonds refer to archived samples (year of sampling indicated
[32]).

FIG. 10. Fallout model used to identify two sources of fallout to the NW Atlantic, namely
Nevada fallout with a low 240Pu/239Pu ratio, but high efficiency for removal into sediments,
and global fallout with a 240Pu/239Pu ratio of 0.18, and low removal to sediments, except in
coastal regions [32].

21
FIG. 11. Vertical profiles of 239,240Pu, 137Cs and 230Th from GEOSECS station G225 in the N
Pacific. Note low Pu/Cs ratios at the surface due to Pu scavenging, higher Pu/Cs at
subsurface Pu maximum, and no detectable Cs below about 2 km, while Pu is found at all
depths. This separation with depth is due to the relative difference between the conservative
nature of Cs in the oceans, and the particle-reactivity of Pu [26].

FIG. 12. Surface ocean concentrations of 137Cs (fCi/kg) in Bikini lagoon in 1972. Note highest
concentrations associated with the testing site and apparent source of Cs to surrounding
waters due to release from coral sediments [37].

22
FIG. 13. Sediment inventory vs. water depth for 239,240Pu and 210Pbexcess in the NW Atlantic.
The dashed line at 100% represents expected delivery of both isotopes [36].

Variability in local sedimentary inventories also tells us something about sediment

redistribution processes, those which could result from storms, or as fine grained sediment are
"focused" or otherwise concentrated in specific physical settings (canyons, deep basins) or are
lost due to slumping along ocean margins or steep inclines. Often, the integrity of deep ocean
box cores can be checked by the presence/absence of fallout Pu or excess natural 210Pb. If
there is core top loss during sampling for example, the uppermost layers which include the
recent fallout signal, would be missing. In general, particle-reactive radionuclides inventories
continue to increase in marine sediment, whereas ocean water concentrations and inventories
decrease due to both dilution and scavenging losses.

4. PACIFIC OCEAN

4.1. Overview

The major source of anthropogenic radionuclides in sea water and sediment in the
Pacific Ocean and its marginal seas can be traced to global and local fallout from nuclear
weapons testing. Other sources have introduced relatively smaller amounts of radionuclides
into the Pacific Ocean.
Past measurements of concentrations of 90Sr, 137Cs and 239,240Pu in surface water, the
water column and sediment from regions of the North and South Pacific Ocean are reported.
A comprehensive collection of published references on these radionuclides in the Pacific
environment is attached (ANNEX IV). The data for concentrations were extracted from these
references as well as from various institutional sources and has been compiled in the
GLOMARD database.

23
 The different regions of the Pacific Ocean were chosen on the basis of known ocean
current systems (Fig. 14), the location of nuclear test sites, the availability of recent data and,
for some, the probability of a relatively uniform distribution of radionuclides.

Radionuclide concentrations measured since 1971 in surface water from 14 regions of

the Pacific Ocean and its marginal seas (Fig. 15) are presented in a series of figures.
Regression analyses of the results provide best estimates of effective half-lives for
radionuclides in surface water. The computed values are used to predict concentrations
expected in surface water in the year 2000 which are compared to the most recently measured
values in the areas concerned and are shown in the related tables. The remaining parts of this
chapter contain tables of data and figures showing recently measured inventories of 90Sr, 137Cs
and 239,240Pu in the water column and in sediment from regions of the NW Pacific. These
results are compared with previous measurements made in the same area to assess changes in
inventory over time.

4.2. Radionuclides in the Pacific Ocean

The behaviour of 90Sr, 137Cs and 239,240Pu in the Pacific Ocean has been discussed in
many papers (see ANNEX IV) and in a more recent review [38]. The most extensive studies
were carried out during the 1973–1974 GEOSECS programme that provided the first
comprehensive dataset on the lateral and vertical distributions of 90Sr, 137Cs and 239,240Pu in
Pacific waters [30]. Traditionally, several Japanese institutes, as well as many other research
groups, have been active in investigating these radionuclides, especially in NW Pacific water
and sediment, e.g. [39–51]. A third group of investigations was concerned with nuclear
weapons testing sites in the Marshall Islands, e.g. [52–54] and French Polynesia, e.g. [55–58].
The behaviour of plutonium in the Pacific Ocean will be discussed in more detail as this
element has received the greatest attention. The state of knowledge of the behaviour of Pu in
the Pacific Ocean has evolved slowly due to the intrinsic complexity of the many factors
involved and to the economic and logistical constraints on its study in the world’s largest
ocean. Three of the main factors relevant to Pu behaviour are:

(i) The physical and chemical form of plutonium as it enters the ocean — frequently
source-dependent,
(ii) The basic physico-chemical properties of plutonium e.g. oxidation state,
speciation and the ability to form complexes, and the resultant phase partition
between particles and solution,
(iii) The physical, chemical and biological processes that act on plutonium in the
Pacific Ocean in a heterogeneous manner — both geographically and over
seasonal, annual and multi-annual time-scales.

The major input of plutonium to the Pacific Ocean both quantitatively and
geographically, resulted from atmospheric testing of nuclear weapons. A significant but
smaller input of plutonium, derives from the global fallout of a 238Pu source in a navigational
satellite (SNAP-9A) that burned up over the Indian Ocean in 1964 [35]. Other inputs, e.g.
from nuclear waste disposal, isolated underwater nuclear tests or land-based releases, are
relatively minor in comparison and tend to have rather localized effects. The primary source
from

24
 FIG. 14. The global surface current system (adapted from The Open University [59]). Cool currents –dashed arrows; warm currents –continuous
arrows. The map shows average winter (Northern hemisphere) conditions.

25
26
80

60

1
40 14
2 3

20
4 5

0 15 6 7

Latitude
8 9
-20
16
10 11
-40
17
12
-60

13
-80
0 20 40 60 80 100 120 140 160 180 200 220 240 260 280 300 320 340 360
Longitude

FIG. 15. Latitudinal boxes in the Pacific and Indian Oceans.

from atmospheric nuclear weapons testing is fallout distributed globally in the stratosphere
and subsequently delivered to land and ocean surfaces through the troposphere. This fallout
pattern has a strong latitudinal dependence with maxima at mid-latitudes and minima towards
the equator and poles [25, 35]. In addition, since the majority of atmospheric nuclear weapons
tests were conducted in the Northern hemisphere, fallout delivery to the Earth’s surface has
been substantially larger than in the Southern hemisphere.

The second and very substantial input of plutonium to the Pacific Ocean was derived
from the extensive series of atmospheric nuclear weapons tests carried out by the US weapons
testing programme at the Pacific Proving Grounds at Bikini (11°36'N, 165°22'E) and
Enewetak (11°30'N, 162°20'E) Atolls between 1946 and 1958 [54]. A total of 66 tests were
conducted at these atolls. Many of these tests were conducted at or near ground level and thus
much of the resultant radioactivity was delivered to the troposphere with substantial fallout to
regional ocean areas. Surface tests conducted over coral islands or over shallow water
produced highly localized input [60] because large quantities of soil were incorporated in the
ensuring fireball and cloud. In these cases different types and sizes of high specific activity
particles were formed consisting of mixtures of partially hydrated CaO, Ca(OH)2 and CaCO3
formed by high temperature vaporisation and subsequent condensation processes [61].
Therefore, in addition to the injection of fallout debris into the stratosphere, these surface-
based tests have produced significant quantities of local, or so-called tropospheric fallout.
Such fallout remains within the troposphere, from which it is rapidly deposited. Depending
upon local wind conditions and wet and dry deposition patterns, tropospheric fallout was
deposited preferentially within the vicinity of the test site [62]. In the years that followed
testing, contaminated particles deposited in lagoon and surrounding slope and basin sediment
formed a reservoir and source term for the marine environment through solubilization and
water transport. The mean exchange rate of Enewetak lagoon water is approximately one
month and estimates for Bikini lagoon water vary between 30 and 140 days [63]. Other
Pacific tests were conducted by the US and the UK at Christmas Island (1°52'N, 157°20'W)
and by the USA at Johnston Atoll (17°00'N, 163°30'W). However, these were conducted at
high altitude and are unlikely to have contributed significantly to local tropospheric fallout in
comparison to the Enewetak and Bikini tests. France also conducted an extensive series of
atmospheric tests at Mururoa and Fangataufa Atolls (around 22°S, 135°W) [57]. Most of the
46 tests and trials were conducted between 1966 and 1974 at altitudes of 200 to 700 m. In
consequence of the much lower yields than of the US tests at Bikini and Enewetak, and the
altitude of detonation, it is anticipated that the delivery of local fallout from the French tests to
the surrounding ocean areas must have been of much smaller significance.

Inventories of 239,240Pu in excess of global fallout levels persisting in Pacific atoll

sediment are continuously mobilised into solution and provide a source term to the
surrounding ocean. Analyses of grab and core samples collected from Enewetak Atoll in 1972
were used to give an estimate of the total sediment inventory for plutonium of 44.4 TBq [52].
The estimated plutonium inventory for Bikini sediment was 54.4 TBq. Using residence times
of lagoon water and the average soluble inventories, it was estimated that the annual discharge
of 239,240Pu from Enewetak and Bikini Atolls is 0.10 and 0.12 TBq, respectively. Thus, the
cumulative export to the equatorial Pacific Ocean over the past 40 years has been about
8 TBq. Typical present-day 137Cs/239,240Pu inventory ratios in the contaminated Marshall
Islands range between 1.8 and 19. This implies that a maximum of about 2 PBq of the present
Pacific Ocean inventory was derived from 137Cs initially deposited on or around the lagoons.
This represents less than 2% of the total 137Cs deposited in the N Pacific Ocean from global
fallout. By comparison, the total 239,240Pu inventory in Mururoa and Fangataufa lagoon
sediment was estimated to be about 25 TBq [58]. For comparison, the 137Cs inventories in

27
sediment in both lagoons are only about 0.9 TBq [57]. Using the radionuclide residence time
of 100 days for Mururoa and 30 days for Fangataufa, the annual release rate for 239,240Pu from
Mururoa and Fangataufa lagoon sediment to the open ocean was estimated to be about
0.01 TBq [57]. Hence, the total cumulative export to the ocean from this source over the past
30 years would be about 0.3 TBq.
A considerable amount of work has been carried out over the last 40 years with respect
to the fate and behaviour of Pu in the Pacific Ocean. For example, [26] included an extensive
section on many aspects of Pu in the Pacific in a major review of the aquatic behaviour of Pu.
Robison and Noshkin [54] have produced an informative review of environmental impact
assessment studies around the US test sites at Bikini and Enewetak, and the IAEA [57]
addressed similar issues around the French test sites at Mururoa and Fangataufa.
The basic property controlling the oceanic behaviour of Pu is its tendency to associate
with particulate phases. This however varies considerably, depending on speciation (e.g.
oxidation state), physico-chemical form and density of particles. The higher oxidation states
(V, VI) would have substantially less particle association than the lower (III, IV), as discussed
in [26]. This was specifically discussed with respect to open Pacific waters in a paper by
Nelson et al. [64]. Buesseler [65] discussed the influence of physico-chemical forms on Pu
oceanic behaviour — noting especially, in the Pacific, the difference between calcium-rich
particles produced following surface tests in the Pacific and the smaller (sub-micron) iron-rich
particles introduced to the stratosphere from atmospheric nuclear weapons tests. Finally,
particle density is a major influence on the oceanic behaviour of Pu. Estuarine, coastal and
slope sediment have been shown in many studies to receive large amounts of scavenged Pu
from the large population of biogenic and inorganic particles present in shallower, near-shore
locations. In contrast, open ocean oligotrophic settings (covering most of the global ocean)
have been shown to exhibit patterns of Pu distributions wherein the largest part of the
delivered Pu is still resident in the water column (e.g. [30, 66]).
In the Pacific, these generally complex patterns are further complicated by substantial
amounts of Pu delivered there, in addition to global fallout, from tropospheric local fallout
from the Bikini and Enewetak test series (such as the "Mike" test in 1952 at Enewetak).
Buesseler [65] has noted that the Pu signal from these tests can be distinguished on the basis
of the much higher proportion of 240Pu relative to 239Pu (see also Chapter 3). Observed
oceanic 240Pu/239Pu ratios of up to 0.36 are contrasted with the value of 0.18 that generally has
represented the global fallout average. Pu from this local fallout, with its characteristic
isotopic signature, has physico-chemical characteristics that lead to its much faster removal
from the ocean surface and transfer to the deep ocean compared to Pu from global fallout. It is
also true that, at the locations where these high ratios were observed, the Pu inventories in the
water column, or total of water plus sediment, are substantially in excess of global fallout
values. The distribution of this excess, both geographically and vertically in the N Pacific is
highly consistent with its originating from a local fallout source because of enhanced
biological removal and the high 240Pu/239Pu signature. The geographical distribution agrees
with that expected from regional input in the vicinity of the test sites, subsequently
redistributed by the Western N Pacific gyral circulation and the Equatorial Current and
Counter-Current systems (Fig. 14). The evidence from vertical distributions can be drawn
from two sets of observations. Firstly, one can look at the distribution of stations that show
elevated Pu concentrations in near-bottom water. Again, the GEOSECS data [30] show deep-
water Pu maxima in the NW Pacific to be well correlated with inventories exceeding global
fallout levels. This has also been seen in other data sets — always subject to data limitations,
such as undersampled deep water or analytical discrepancies. Secondly, it is useful to examine
the geographical distribution of locations where data permit an assessment of the proportion

28
of Pu inventories between the water column and underlying sediment — or even between
upper and deep ocean water inventories. A higher proportion of the total Pu inventory was
found at stations of high sediment Pu inventories in the western N Pacific (up to 16%)
compared to the station north of Hawaii (2%). Taken together, these observations seem to
point to the existence, in the Pacific, of a second source of Pu (in addition to global fallout),
derived from the ground level nuclear tests in the 1950s, which has been shown to be
associated with particle scavenging and transport processes at rates substantially greater than
the rates typically seen for global fallout Pu in open ocean regions.

4.3. Distribution of radionuclides in surface water and sediment

For the study of the distribution of radionuclides in sea water and sediment, the Pacific
Ocean has been divided into different latitudinal boxes (Fig. 15) on the basis of known ocean
current systems, the location of nuclear test sites, the availability of recent data and, the
probability of a relatively uniform distribution of some radionuclides. Twelve boxes have
been delineated in the Pacific Ocean and one box has been attributed to the Southern Ocean.
The Sea of Japan has been given a separate box because of its oceanographic specificity and
importance in marine radioactivity studies. Box 1 (north of 40°N) is the subarctic Pacific
Ocean, where the largest fallout rates of 137Cs and 90Sr over the Pacific Ocean were observed
in the 1960s [2]. Boxes 2 and 3 (25°–40°N) are upstream and downstream of the Kuroshio
Extension, respectively, where the water masses of the Kuroshio and Oyashio Currents mix.
Boxes 4 and 5 (5°–25°N) are downstream and upstream of the North Equatorial Current,
which is a typical oligotrophic ocean current corresponding to the subtropical gyre (Box 5
also includes the California Current). These boxes include the Pacific Proving Grounds
nuclear weapons tests sites (Bikini, Enewetak, Johnston Atolls and others), especially
important for plutonium [65, 67]. The subtropical region of the western N Pacific was
affected by local fallout as opposed to the subtropical region of the eastern N Pacific. Boxes 6
and 7 (5°S–5°N) are downstream and upstream of the South Equatorial Current, respectively.
The boundary between boxes 4, 5 and 6, 7 is approximately at the Equatorial Counter-
Current. Box 7 includes the Equatorial upwelling region. Boxes 8 and 9 (5°–25°S) are
downstream and upstream of the South Equatorial Current, respectively. The boundary
between boxes 6, 7 and 8, 9 approximately corresponds to the South Equatorial Counter-
Current. Box 9 includes the French nuclear weapons test sites (Mururoa and Fangataufa).
Box 10 (25°–40°S) corresponds to the Tasman Sea. Box 11 (25°–40°S) is the mid-latitude
region of the South Pacific. Boxes 12 (40°–60°S) and 13 (below 60°S) include the Southern
Ocean and the Antarctic Circumpolar Current.

4.3.1 Surface water

Figures 16 to 19 show 3H, 90Sr, 137Cs and 239,240Pu surface water data from the
GLOMARD database for the period 1991–1995, for which average radionuclide
concentrations were calculated for the corresponding latitudinal boxes in the Pacific Ocean.
Although the density of data is not very high, a clear latitudinal effect of increasing average
radionuclide concentrations from the south to the north can be observed, as expected. The 3H
data have a very good coverage in the central and South Pacific Ocean thanks to the WOCE
programme [68]. The average concentrations increase from 13 mBq/L estimated for Box 13,
up to 330 mBq/L estimated for the Sea of Japan. 90Sr data have the highest density in the NW
Pacific Ocean (similar to 137Cs and 239,240Pu) increasing from 0.4 mBq/L from the south to 1.8
mBq/L for the Sea of Japan. 137Cs and 239,240Pu data show an increase from 0.6 mBq/L and 0.8
μBq/L, respectively, in the south to 2.8 mBq/L and 8.5 μBq/L in the Sea of Japan,
respectively.

29
 Except for the fact that the highest average radionuclide concentrations were observed
in the Sea of Japan, the data show lower average concentrations than expected in Box 3 for
239,240
Pu (however, the data set is very small). Similarly, in the north, Box 1 shows lower
average concentrations for 137Cs than expected (however, the geographical distribution of data
in this box is heavily concentrated in the NW).
Similar data sets are shown in Figs 20 to 23 for the years 1996–2000. Here, the data are
very sparse and they are mainly based on the results obtained in the framework of the
WOMARS project. A comparison (where possible) of decay-corrected data shows more or
less the same trend in data observed for the years 1991–1995.
Although the data density is very low, it was possible, at least for the NW Pacific
Ocean, to develop a distribution chart for 137Cs in surface water using data extracted from the
GLOMARD database for the years 1991–2000 (decay-corrected to 1.1.2000 (Fig. 24)).
For a more detailed discussion on radionuclide data in the boxes see Chapter 4.3.
4.3.2. Sediment

A similar set of data was developed for the distribution of 90Sr, 137Cs and 239,240Pu in
sediment (Figs 25 to 27 for 1991–1995 and Figs 28 to 29 for 1996–2000 (no data are
available for 239,240Pu)). The data density is even less than for surface water. Only few data are
available for the NW Pacific Ocean and the Sea of Japan, mainly obtained in the framework
of the WOMARS project. Therefore, a detailed evaluation of sediment data is not possible.

Pacific sediment is, of course, the ultimate sink for the Pu present there. The sheer size
and great depth of the Pacific have limited the number of Pacific sediment studies. However,
shelf and slope studies have been undertaken on both the eastern and western Pacific margins
due to their proximity to coastal laboratories. On the eastern side, Sholkovitz [26] has
presented a comprehensive overview of previous work on California basin sediment. Beasley
et al. [69] reported on transuranic measurements in shelf sediment off Washington and
Oregon. Some data were reported for the western side [70], the East China and Yellow Seas
[43] and the Seto Inland Sea [71]. All these studies point to the same major conclusion. As
indicated by the general excess inventories over those anticipated from global fallout, Pacific
marginal sediment underlying waters with high biological productivity and larger suspended
sediment loads are major sinks in Pu removal and sequestration. The additional component
from transported local fallout Pu has also to be considered in respect of western marginal
sediment — as discussed in Chapter 4.6.2.

The number of open Pacific Ocean sediment Pu studies is smaller than needed to permit
a comprehensive estimate of the distribution and inventories residing there — especially for
specific points in time. For example, it is unfortunate that the comprehensive GEOSECS
sampling programme did not collect sediment cores at the wide distribution of stations
occupied. There is another factor that complicates the acquisition of reliable estimates of Pu
distributions and inventories, the heterogeneity of the observed Pu distributions to be found
— especially in deep-ocean sediment. This is presumably a consequence of the relatively
short time, in a geological sense, over which Pu has been arriving at the sea-floor.
Presumably, on the scale of hundreds and thousands of years, these distributions will tend to
even out — beginning to approach the more homogeneous distributions at a steady state that
can be observed for long lived Th isotopes, for example [72]. There, in a series of 17 sediment
cores collected in the late 1970s in a single area in the central N Pacific Ocean, north of
Hawaii

30
 80

60

330±170 210±70
(13) (5)

40
165±12 177±12
(3) (4)

20
112±17
(26)
Latitude

0 84±16
(26)

75±20
(44)
-20
54±13
71±6
(15) (69)
-40
35±3
(19)

-60
13±1
(3)

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 16. 3H in surface water (1991–1995), decay-corrected to 01.01.2000, in mBq/L.

80

60

1.8±0.4
(167) 1.8±2.7
(64)
40
1.7±0.5 1.41±0.07
(115) (3)

20 1.61±0.18
(4) 1.12±0.15
(5)
Latitude

1.46±0.05 1.05±0.11
0 (2) (3)

1.19 1.03±0.10
(1) (12)

-20

0.6±0.3
(4)
-40
0.37±0.03
(2)

-60
0.10 (1)

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 17. 90Sr in surface water (1991–1995), decay-corrected to 01.01.2000, in mBq/L.

31
 80

60

2.7±0.5 2.3±0.6
(250) (66)
40
2.7±0.6 2.8±0.5
(158) (3)

20 2.7±0.6 2.3±0.3
(14) (4)
Latitude

2.32±0.11 1.86±0.12
0 (2) (3)

1.67 1.91±0.14
(1) (12)

-20

1.1±0.6
(4)
-40
0.57±0.02
(2)

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 18. 137Cs in surface water (1991–1995), decay-corrected to 01.01.2000, in mBq/L.

80

60

8.5±5.8
(71) 5.3±5.0
(10)
40
5.5±2.4 0.71±0.13
(25) (3)

20 3.4±1.4 1.7±0.7
(20) (5)
Latitude

2.7±0.2
0 3.6±2.7 (3)
(5)
1.5±1.2 4.7±5.5
(5) (28)

-20
1.9±0.8
(5) 1.6±0.6
(4)
-40
0.82
(1)

-60
1.33 (1)

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 19. 239,240Pu in surface water (1991–1995) in μBq/L.

32
 80

60

40
136±8
(8)

20 109±7
(10)
Latitude

0
89±4
(3)

-20

122
(1)
-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 20. 3H in surface water (1996–2000), decay-corrected to 01.01.2000, in mBq/L.

80

60

1.6±0.3
(42) 1.31±0.3
(3)
40 1.6±0.3
(31)

20 1.50±0.09
(13)
Latitude

0
1.08±0.02
(4)

-20

0.8±0.2
(3)
-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude
90
FIG. 21. Sr in surface water (1996–2000), decay-corrected to 01.01.2000, in mBq/L.

33
 80

60

2.8±0.5
(44) 2.0±0.5
(4)
40 2.4±0.5
(30)

20 2.4±0.4
(8)
Latitude

1.72±0.08
(4)
-20
1.38±0.09
(3)

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 22. 137Cs in surface water (1996–2000), decay-corrected to 01.01.2000, in mBq/L.

80

60

6.6±2.5
(30) 7.8±8.7
(2)
40
3.8±2.4
(6)

2.4±0.7
20 (7)
Latitude

0
5.6±1.9
(4)

-20
4.33±0.06
(2)

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 23. 239,240Pu in surface water (1996–2000), in μBq/L.

34
 FIG. 24. 137Cs in surface water of the NW Pacific Ocean (1991–2000).

80

60
0.2 ± 0.2
(41) 0.3 ± 0.1
(4)
40
0.1 ± 0.1
(12)

20
Latitude

-20

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 25. 90Sr in NW Pacific surface sediment (1991–1995), decay-corrected to 01.01.2000,

Bq/kg dw.

35
Hawaii, Bowen reported variations of around a factor of 10 in the observed Pu distributions
and inventories. In a similar manner, the depths of bioturbation varied considerably — from 5
to 20 centimetres. Although sampling artefacts are always a concern, he reported that this was
not a major contributor to the observed heterogeneity as four different sampling devices were
used and no clear correlation with device was found. The hypothesis advanced to explain this
heterogeneity was based on the linkage, over short time intervals, with the variability in the
places of more intense bioturbation — given the relatively small population density of benthic
organisms supportable by low fluxes of food via sinking particles.
Even with this limitation, the actual number of places where deep ocean Pacific Pu
measurements in sediment have been obtained is quite limited with respect to spatial coverage
— and even more so in respect of time. The main data sets built into the Global Marine
Radioactivity Database (GLOMARD) at IAEA-MEL [73] were supplied by these Japanese
institutions: the Japan Chemical Analysis Center (JCAC), the Marine Safety Agency (MSA)
and the Fisheries Agency (FA). IAEA-MEL data from the joint Japanese-Korean-Russian
expeditions in 1994 [74] and 1995 [75] were used in the evaluations as well [76, 77]. Further
data were obtained from a literature survey covering the western and central N Pacific [41, 42,
44–48, 78–82] as well as the eastern Equatorial Pacific [83]. A significant trend, discussed
below, is the frequently observed excesses of Pu, in either absolute or relative (to 137Cs) terms
found especially in western regions close to downstream locations around the test sites at
Bikini and Enewetak and towards the equator in the eastern Pacific. This will be discussed
with reference to the important Pu source from local fallout from these atoll weapons tests.
4.4. Surface water radionuclide time series

This section compares 90Sr, 137Cs and 239,240Pu concentrations measured since 1971 in
surface water of 14 regions of the Pacific Ocean and its marginal seas in a series of figures.
Regression analyses of the results provide best estimates of effective decay constants and
effective half-lives for radionuclides in surface water. The computed values are used to
predict concentrations in surface water for the year 2000 and are compared to the most
recently measured values in the areas concerned. Levels of anthropogenic radionuclides
(137Cs, 90Sr and 239,240Pu) in surface water of the Pacific Ocean were evaluated using the data
stored in the GLOMARD database.
The time series of anthropogenic radionuclides (90Sr, 137Cs and 239,240Pu) during 1971–1998
are examined to estimate their surface concentrations in the year 2000, as anthropogenic
radionuclides in surface water in the 1950s and 1960s were mainly controlled by input
processes such as global and local fallout [2]. The concentrations of 90Sr with time in surface
water for each box decrease exponentially (Figs 30 to 33). Therefore, temporal changes in
surface radionuclide concentrations can be expressed by an exponential function over three
decades in time. The surface concentrations and effective half-lives of 137Cs, 90Sr and 239,240Pu
in each box of the Pacific are calculated from the corresponding regression lines. However,
the confidence levels of regression lines vary greatly between boxes because of the different
densities of data.
The 90Sr concentrations in surface water in 2000 calculated from the time series or
estimated from recent measurements are in the range of 0.4 to 1.5 mBq/L (Table VI). The
surface concentration of 90Sr in Boxes 8, 10, 11 and 12 cannot be estimated because of the
lack of data (less than 3 values). Most of the surface 90Sr concentration data are crowded in
Box 2 (76%). Higher surface 90Sr concentration occurs in the mid-latitude region of the
western N Pacific (Box 2). The lowest values appear in regions of high latitude in the South
Pacific. The geographical distribution of 90Sr in Pacific surface water in 2000 is
homogeneous, as is that of 137Cs.

36
 80

60
2.5 ± 2.3
(66) 2.9 ± 1.1
(13)
40
2.2 ± 1.8
(41)

20
Latitude

-20

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 26. 137Cs in NW Pacific surface sediment 1991–1995, decay-corrected to 01.01.2000,

Bq/kg dw.

80

60
0.3 ± 0.4
(43) 0.6 ± 0.4
(10)
40
0.3 ± 0.5
(17)

20
Latitude

-20

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 27. 239,240Pu in NW Pacific surface sediment (1991–1995), decay-corrected to

01.01.2000, Bq/kg dw.

37
 80

60
0.4 ± 0.2
(9)
0.7 ± 0.7
40 (3)

0.1
(1)

20
Latitude

-20

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 28. 90Sr in NW Pacific surface sediment (1996-2000), decay-corrected to 01.01.2000,

Bq/kg dw.

80

60
3.0 ± 1.7
(27) 4.0 ± 1.2
(7)
40
2.8 ± 1.9
(12)

20
Latitude

-20

-40

-60

-80
100 120 140 160 180 200 220 240 260 280
Longitude

FIG. 29. 137Cs in NW Pacific surface sediment (1996–2000), decay-corrected to 01.01.2000,

Bq/kg dw.

38
 The calculated 137Cs concentrations in surface water for each box in 2000, together with
the most recent data are shown in Table VII and Figs 34 to 37. The surface concentration of
137
Cs in Boxes 8 and 12 cannot be estimated because of the lack of data (less than 3 values).
The 137Cs concentrations ranged from 0.7 to about 2.8 mBq/L. Higher surface 137Cs
concentration occurs in the eastern Equatorial Pacific (Box 7). Lower values appear in the
Tasman Sea (Box 10). The geographical distribution of surface 137Cs in 2000 differed from
that observed in the 1960s. The geographical distribution of surface 137Cs in the early 1970s
showed maxima in the mid-latitude region of the N Pacific [84], when it was still controlled
by the input process, i.e., global fallout. Occurrence of higher surface 137Cs concentration in
the eastern Equatorial Pacific may be explained by the south-westward advection of
subsurface higher 137Cs concentrations penetrating in the eastern N Pacific and the upwelling
of subsurface 137Cs in the Equatorial Pacific [85, 86]. In fact, the subsurface maximum of
137
Cs concentrations (near 100 m depth) has been observed in the subtropical N Pacific [30,
46]. It is noteworthy that surface 137Cs is homogeneous in the Pacific compared to surface
239,240
Pu.

The 239,240Pu concentrations in surface water in 2000 (Figs 38 to 41) are estimated to be
in the range of 0.5 to about 3 μBq/L (Table VIII). Higher surface 239,240Pu concentrations
appear in the subarctic Pacific (Box 1) and the eastern Equatorial Pacific (Box 7). Higher
surface 239,240Pu concentration in the subarctic Pacific can be explained by rapid recycling of
scavenged 239,240Pu due to large vertical mixing in winter, whereas higher surface 239,240Pu in
the eastern Equatorial Pacific is supported by upwelling of subsurface enriched 239,240Pu as
well as 137Cs. The lower values appear in the mid-latitude region of the eastern N Pacific (Box
3), which is consistent with the higher decrease rate of 137Cs in Box 3. Another point is that
estimated surface 239,240Pu concentrations in Boxes 2 and 4 of the western N Pacific are higher
than those in Boxes 3 and 5 of the eastern N Pacific. Furthermore, there is only a small
difference in surface 239,240Pu concentrations between the mid-latitude regions of the Northern
and Southern hemispheres. As a result, the current geographical distribution of 239,240Pu
concentrations in surface water of the Pacific is very complex as it is controlled by both
biogeochemical and physical processes [30, 49].
Therefore one may conclude that the present concentrations of anthropogenic
radionuclides (90Sr, 137Cs and 239,240Pu) in Pacific surface water are controlled by
oceanographic processes (horizontal advection, vertical mixing and biogeochemical
processes) rather than input processes due to global fallout.
In order to assess the environmental effects of anthropogenic radionuclides, it is
important to estimate the effective half-lives (residence times) of 90Sr, 137Cs and 239,240Pu in
each box. They have been calculated from their corresponding regression lines and the results
are summarized in Tables VI to VIII. The effective half-life of 137Cs in surface water in each
box ranged from 11 to about 30 years. The shortest effective half-life of 137Cs is observed in
the mid-latitude of the eastern N Pacific (Box 3).

39
TABLE VI. 90Sr EFFECTIVE HALF-LIVES AND CONCENTRATIONS IN SURFACE
WATER FOR THE YEAR 2000
Box Effective Est. concentration Recent measurements Decay-corr.
No. half-life in 2000.01.01 value to
T1/2 ± 1σ Concentration ± 1σ Averaged No of Period 2000.01.01
(years) (mBq/L) value data (mBq/L)
(mBq/L)
01 16.2 ± 1.5 1.3 ± 0.1 1.5 ± 0.3 3 1996–1997 1.3
02 14.4 ± 0.7 1.1 ± 0.1 1.7 ± 0.4 31 1996–1997 1.6
03 10.1 ± 0.5 1.0 ± 0.1 1.7 ± 0.1 3 1993 1.4
04 15.0 ± 1.4 1.2 ± 0.1 1.6 ± 0.1 13 1997 1.5
05 14.0 ± 1.4 0.9 ± 0.1 1.3 ± 0.2 5 1993 1.1
06 21.4 ± 2.0 1.5 ± 0.1 1.7 ± 0.1 2 1993 1.5
07 19.6 ± 5.0 1.0 ± 0.3 1.2 ± 0.1 3 1993 1.1
08 1.4 ± 0.2 1 1993 1.2
09 17.9 ± 1.2 1.0 ± 0.1 1.2 ± 0.1 4 1996 1.1
10 0.9 ± 0.2 3 1998 0.8
11 0.8 ± 0.4 4 1993 0.6
12 0.4 ± 0.1 2 1993 0.4
13 0.1 ± 0.1 1 1994 0.1
14 14.1 ± 0.6 1.4 ± 0.1 1.8 ± 0.3 42 1996–1997 1.6
15 1.1 ± 0.2 15 1998 1.0
16 1.2 ± 0.2 7 1998–1999 1.1
17 0.7 ± 0.4 12 1998–1999 0.7
18 13.3 ± 1.4 1.6 ± 0.2 2.4 ± 0.4 1 1997 2.3
19
20 5.8 ± 0.5 1.5 ± 0.1 2.0 ± 0.5 7 1997 1.9
21 12.0 ± 1.7 8.9 ± 1.3 12.0 ± 3.1 71 1996–1997 11.1
22 6.9 ± 0.4 2.9 ± 0.2 4.3 ± 1.3 118 1996–1999 4.0
23 49 ± 84 14 1999 49
24 5.3 ± 0.7 2.6 ± 0.3 4.5 ± 1.6 43 1996–1997 4.1
25 25.8 ± 3.4 1.5 ± 0.2 2.2 ± 0.9 17 1996–1999 2.1
26 22 ± 4.0 15 1995–2000 17
27 1.8 ± 0.3 15 1997–1998 1.7
28 13.8 ± 1.4 0.7 ± 0.1 1.3 ± 0.7 17 1996–1998 1.2
29 24.2 ± 2.1 0.8 ± 0.1 1.0 ± 0.1 5 1992–1993 0.8
30 17.3 ± 8.8 0.3 ± 0.2 0.5 ± 0.2 2 1993 0.4

40
 Box 01 Box 02
100 100

10 10

Sr (mBq/L)

Sr (mBq/L)
1

90

90
1

0.1
0.1 1950 1960 1970 1980 1990 2000
1950 1960 1970 1980 1990 2000
Year Year

Box 03 Box 04
100 1000

100
10

10
Sr (mBq/L)

Sr (mBq/L)
90

90
1
1

0.1
0.1
1950 1960 1970 1980 1990 2000
1950 1960 1970 1980 1990 2000
Year Year

FIG. 30. 90Sr in Pacific surface water.

41
42
Box 05 Box 06
100 100

10 10

Sr (mBq/L)
Sr (mBq/L)

90
1

90
1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 07 Box 08
100 100

10 10

Sr (mBq/L)
Sr (mBq/L)

90
1
90
1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 31. 90Sr in Pacific surface water.

 Box 09 Box 10
100 100

10 10

Sr (mBq/L)

Sr (mBq/L)
90

90
1 1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 11 Box 12
100 100

10 10

Sr (mBq/L)

Sr (mBq/L)
90
1

90
1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 32. 90Sr in Pacific surface water.

43
 Box 13
100

Sr (mBq/L)
10

90
1

0.1
1950 1960 1970 1980 1990 2000
Year

FIG. 33. 90Sr in Pacific surface water.

TABLE VII. 137Cs EFFECTIVE HALF-LIVES AND CONCENTRATIONS IN SURFACE
WATER FOR THE YEAR 2000
Box Effective Estimated Recent measurements Decay-
No. half-life concentration corrected
in 2000.01.01 value to
T1/2 ± 1σ Concentration ± 1σ Averaged value Number of Period 2000.01.01
(years) (mBq/L) (mBq/L) data (mBq/L)
01 13.7 ± 0.8 1.7 ± 0.1 2.1 ± 0.5 4 1996–1997 2.0
02 16.5 ± 0.9 2.3 ± 0.1 2.6 ± 0.6 30 1996–1997 2.4
03 10.6 ± 0.5 1.9 ± 0.1 3.2 ± 0.6 3 1993 2.8
04 24.2 ± 3.1 2.8 ± 0.4 2.6 ± 0.4 7 1997 2.4
05 18.4 ± 4.2 2.7 ± 0.6 2.7 ± 0.4 4 1993 2.3
06 29.9 ± 7.7 2.4 ± 0.6 2.7 ± 0.1 2 1993 2.3
07 21.3 ± 3.0 1.7 ± 0.2 2.2 ± 0.1 3 1993 1.9
08 1.9 ± 0.4 1 1993 1.7
09 28.5 ± 1.6 1.8 ± 0.1 1.9 ± 0.1 4 1996 1.7
10 23.3 ± 2.6 1.3 ± 0.1 1.4 ± 0.1 3 1998 1.4
11 11.9 ± 2.0 0.7 ± 0.1 1.3 ± 0.8 4 1993 1.1
12 0.6 ± 0.3 2 1993 0.6
13 0.1 ± 0.1 1 1994 0.1
14 19.0 ± 0.9 2.5 ± 0.1 3.0 ± 0.5 44 1996–1997 2.8
15 20.2 ± 1.9 1.5 ± 0.1 1.6 ± 0.3 17 1998 1.6
16 26.3 ± 4.9 1.9 ± 0.4 2.2 ± 0.3 7 1998–1999 2.1
17 12.7 ± 7.0 0.7 ± 0.4 1.1 ± 0.6 12 1998–1999 1.0
18 13.6 ± 1.5 2.8 ± 0.3 15 ± 3 1 1997 14
19 0
20 4.2 ± 0.2 1.9 ± 0.1 3.8 ± 2.1 9 1997 3.6
21 14.1 ± 1.8 49.8 ± 6.5 66 ± 20 214 1996–1997 61
22 5.7 ± 0.3 4.5 ± 0.2 6.9 ± 3.1 137 1996–1999 6.5
23 57 ± 55 28 1999 57
24 6.9 ± 0.6 3.1 ± 0.3 4.5 ± 1.6 44 1996–1997 4.2
25 23.3 ± 1.8 2.3 ± 0.2 4.5 ± 2.9 15 1996–1999 4.2
26 7.3 ± 1.2 25 ± 3 30 ± 14 20 1996–2000 25
27 2.7 ± 0.4 15 1997–1998 2.6
28 14.9 ± 1.6 1.3 ± 0.1 1.8 ± 0.9 16 1996–1997 1.7
29 23.7 ± 5.7 1.4 ± 0.3 1.7 ± 0.2 5 1991–1993 1.4
30 20.2 ± 6.3 0.5 ± 0.1 0.7 ± 0.2 2 1993 0.6

44
 Box 01 Box 02
1000 100

100
10

10

Cs (mBq/L)

Cs (mBq/L)
1

137

137
1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 03 Box 04
100 1000

10 100

Cs (mBq/L)

Cs (mBq/L)
1 137
10

137
0.1 1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 34. 137Cs in Pacific surface water.

45
46
Box 05 Box 06
100 100

10 10

Cs (mBq/L)
Cs (mBq/L)
1 1

137
137
0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 07 Box 08
100 100

10 10

Cs (mBq/L)
Cs (mBq/L)
1 1

137
137

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 35. 137Cs in Pacific surface water.

 Box 09 Box 10
100 10

10

Cs (mBq/L)

Cs (mBq/L)
1

137

137
0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 11 Box 12
100 100

10 10

Cs (mBq/L)
1 Cs (mBq/L) 1

137
137

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 36. 137Cs in Pacific surface water.

47
 Box 13
100

Cs (mBq/L)
10

137

0.1
1950 1960 1970 1980 1990 2000
Year

FIG. 37. 137Cs in Pacific surface water.

The longest effective half-life of 137Cs is found in the Equatorial Pacific (Boxes 6
and 7), (which may be due to Equatorial upwelling) and in the eastern subtropical South
Pacific (Box 9). The effective half-life of 90Sr in surface water in each box ranged from 10 to
21 years. The shortest effective half-life of 90Sr is observed in the eastern N Pacific (Box 3).
The longest effective half-life of 90Sr occurs in the Equatorial Pacific (Boxes 6 and 7), which
is the same area as for 137Cs. The effective half-life of 90Sr in seems to be a little less than that
of 137Cs, however the data are not precise enough to confirm this. The effective half-life of
239,240
Pu in surface water in each box ranged from 5 to about 15 years. The shortest effective
half-life of 239,240Pu is observed in the mid-latitude region of the eastern N Pacific (Box 3) as
for 137Cs.
These findings suggest that the mid-latitude region of the eastern N Pacific is a sink of
anthropogenic radionuclides. The surface water mass in the mid-latitude region of the eastern
N Pacific is penetrated under the surface layer of the subtropical gyre. As a result, the
subsurface maximum of 137Cs is formed in the subtropical N Pacific [30, 85]. The longest
effective half-life of 239,240Pu is found in the eastern Equatorial Pacific (Box 7), as is the case
for 137Cs and 90Sr. At present, the eastern Equatorial Pacific seems to behave as a source of
anthropogenic radionuclides. The effective half-life of 239,240Pu is generally shorter than that
of 137Cs in each box. Plutonium is a particle-reactive radionuclide as opposed to 137Cs i.e.
plutonium reacts with biogenic particles in surface water [67, 87], sinks with attached
particles, and is remobilised as a result of the biological decomposition of particles in deeper
water [49].
In South Pacific surface water, the effective half-lives of the radionuclides investigated
appear to be longer than in the N Pacific. When corrected for radioactive decay, surface 137Cs
in the South Pacific (except for Box 11) has gradually increased over the past three decades.
This may suggest that 137Cs in the N Pacific is transported to the S Pacific, because the major
input of 137Cs due to global and local fallout occurred in the N Pacific.

When the 90Sr data for the North, Equatorial and South Pacific are grouped (Table IX),
the corresponding mean effective half-lives are 12 ± 1, (North) 18 ± 2 (South) and 21 ± 2
years (Equatorial Pacific). All Pacific data together give an effective half-life of 90Sr of 16 ± 2
years. 137Cs and 239,240Pu effective half-lives for the whole Pacific Ocean are 16 ± 4 and 7 ± 1
years, respectively.

48
TABLE VIII. 239,240Pu EFFECTIVE HALF-LIVES AND CONCENTRATIONS IN
SURFACE WATER FOR THE YEAR 2000

Box Effective Est. Recent measurements

No. half-life concentration
in 2000.01.01
T1/2 ± 1σ Concentration ± Averaged value Number of Period
(years) 1σ (μBq/L) (μBq/L) data
01 16.7 ± 4.3 2.8 ± 0.7 7.9 ± 8.7 2 1996–1997
02 9.3 ± 1.4 2.2 ± 0.3 3.8 ± 2.4 6 1996–1997
03 5.1 ± 0.7 0.5 ± 0.1 0.7 ± 0.1 3 1993
04 7.2 ± 0.7 1.6 ± 0.2 2.4 ± 0.7 7 1997
05 8.4 ± 1.5 0.9 ± 0.2 1.7 ± 0.7 2 1993
06 9.0 ± 2.0 1.3 ± 0.3 3.6 ± 2.7 5 1991–1994
07 15.1 ± 4.2 1.9 ± 0.5 2.7 ± 0.2 3 1993
08 1.5 ± 1.2 5 1992–1993
09 12.1 ± 3.6 1.6 ± 0.5 5.7 ± 1.4 4 1996
10 4.3 ± 0.1 2 1998
11 1.6 ± 0.6 4 1993
12 0.8 ± 0.5 1 1993
13 14.1 ± 7.1 1.0 ± 0.5 1.3 ± 0.7 1 1994
14 15.7 ± 2.6 5.2 ± 0.9 6.6 ± 2.5 30 1996–1997
15 21.2 ± 7.6 1.5 ± 0.5 1.9 ± 1.2 13 1998
16 12.9 ± 5.3 2.2 ± 0.9 3.0 ± 1.5 4 1998–1999
17 8.6 ± 1.1 0.8 ± 0.1 1.0 ± 0.5 10 1998–1999
18 13.2 ± 1.5 5.0 ± 0.5 6.4 ± 1.5 24 1995
19
20 20 ± 12 7 1997
21 4.9 ± 1.4 1.6 ± 0.5 3.4 ± 2.5 21 1996
22 24 ± 17 11 ± 8 15 ± 10 33 1997
23 500 ± 400 1994–1999
24 6.9 ± 1.2 9.5 ± 1.7 13 ± 8 18 1997
25 12.8 ± 2.5 5.1 ± 1.0 36 ± 16 9 1997
26 5.3 ± 2.3 5 2000
27 14 ± 4 7 1997–1998
28 8.8 ± 0.6 3.1 ± 0.2 5.0 ± 2.7 17 1996–1998
29 9.8 ± 2.9 1.5 ± 0.5 2.8 ± 1.3 5 1993
30 10.7 ± 4.9 1.1 ± 0.5 1.8 ± 0.6 1 1993

49
50
Box 01 Box 02
100 100

10
10

Pu (µBq/L)

Pu (µBq/L)
1

239+240

239+240
0.1

0.1 0.01
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 03 Box 04
100 1000

10 100

Pu (µBq/L)
1 Pu (µBq/L) 10

239+240
239+240

0.1 1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 38. 239,240Pu in Pacific surface water

 Box 05 Box 06
100 100

10 10

Pu (µBq/L)

Pu (µBq/L)
1 1

239+240

239+240
0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 07 Box 08
100 100

10 10

Pu (µBq/L)
Pu (µBq/L)
1 1

239+240
239+240

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 38. 239,240Pu in Pacific surface water

51
52
Box 09 Box 10
100 100

10 10

Pu (µBq/L)
Pu (µBq/L)
1 1

239+240
239+240
0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 11 Box 12
100 100

10 10

Pu (µBq/L)
1 Pu (µBq/L) 1

239+240
239+240

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 40. 239,240Pu in Pacific surface water

 Box 13
100

Pu (µBq/L)
10

239+240
1

0.1
1950 1960 1970 1980 1990 2000
Year

FIG. 41. 239,240Pu in Pacific surface water.

90 137 239,240
TABLE IX. MEAN EFFECTIVE HALF-LIVES OF Sr, Cs AND Pu IN PACIFIC
OCEAN SURFACE WATER

Effective Half-life ± 1σ* (years)

90 137 239,240
Area Boxes Sr Cs Pu
North Pacific 01-05 12.4 ± 1.1 12.7 ± 1.4 6.7 ± 0.9
Equatorial Pacific 06-07 21.1 ± 1.9 28.6 ± 3.0 10.2 ± 2.4
South Pacific 08-12 17.9 ± 1.0 22.2 ± 5.2 12.1 ± 3.6
All Pacific 01-12 15.9 ± 2.4 15.9 ± 4.3 7.4 ± 1.1

* Error weighted averaged values

4.5. Water column radionuclide time series

The primary focus of work to date has been on the distribution and behaviour of 90Sr,
137
Cs and 239,240Pu in the water column. Bowen et al. [30] have made the most comprehensive
study of these radionuclides in open Pacific waters. This study presented and discussed the
data obtained at 29 stations in 1973–74 as part of the GEOSECS programme. They covered
much of the N Pacific but did not go further south than 19°S. So, as in other studies, the South
Pacific has received little attention.
A number of other studies have been made subsequent to the GEOSECS study e.g. [41,
42, 45–48, 51, 78, 81, 82, 88, 89]. These studies provide data to augment the GEOSECS data
and to compare possible changes with time in the distributions and inventories in the water
column. Some comparative observations are made below.

Most stations in the Pacific Ocean visited in 1973 during the GEOSECS expedition
provided 90Sr, 137Cs and Pu water profile data with high spatial and depth resolutions [30].
Therefore, one of the objectives of the IAEA 1997 expedition to the NW Pacific Ocean
carried out in the framework of the WOMARS project was to re-visit some of the GEOSECS
stations so that the development of radionuclide concentrations in the water column and their
distribution could be evaluated with time. A similar comparison is possible with the data

53
obtained by the KNORR-1978 [82] and Hakuho Maru 1980, 1982 [41, 80] expeditions. The
data compiled from these four expeditions, as well as data from other expeditions to the
region, enabled the development of time series for studying the behaviour of radionuclides in
the ocean with time over the past 24 years. Figure 42 shows the main sampling stations in the
NW Pacific Ocean for which the radionuclide time series will be compared. However, the
general evaluation of radionuclide data in the Pacific was done using a much larger data set
collected and stored in GLOMARD.

Figures 43 to 46 and 47 to 50 show 90Sr and 137Cs profiles, respectively, in water

columns of the central NW Pacific Ocean at GEOSECS, Hakuho Maru and IAEA stations
(the positions of the sampling stations are shown in Fig. 42). When comparing for instance
Figs 43 (90Sr) and 47 (137Cs), it can be seen that both radionuclides show similar behaviour,
except that 137Cs concentrations are higher by a factor of about 1.6, which represents the
typical global fallout ratio for these radionuclides. There is a remarkable decrease in surface
and subsurface concentrations from the GEOSECS to the IAEA expeditions –from about 3 to
2 Bq/m3 (peak values) for 90Sr (Fig. 43) and from about 4 to 3 Bq/m3 for 137Cs (Fig. 47).

Oceanic studies of the behaviour of Pu have indicated that, especially in major low
productivity oceanic areas, it is clearly not being as rapidly transferred to sediment as more
reactive actinides such as Th or Am. Nevertheless, the particulate associations in transport to
sediment and retention there, is an important aspect of Pacific Pu studies and a number of
papers have addressed this. For example, at least two studies involving sediment traps [89,
90] have served to confirm that, as in other oceans, the flux of sinking biogenic particles fed
by biological production in the surface ocean, is the major vehicle for the transport of Pu (or
other reactive elements) from the surface to the deep ocean. Clearly, Pu enters into the cycle
of organic material that sinks from the surface ocean. On its descent, this material is exposed
to oxidation and bacterial degradation processes and both the organic material and its
associated elements or radionuclides are to some extent released into sea water. As has been
widely recognized, only a very small fraction (in the one per cent range) of material
originating at the surface actually arrives at the sea-floor. This process is clearly responsible
for the observed deep-water Pacific distributions of Pu below depths ventilated physically
from the surface. Furthermore, such material delivered to the sea-floor is available for mixing
by benthic organisms into bottom sediment, and can also be released to overlying waters by
oxidation prior to burial. The latter process can be expected to produce the bottom Pu maxima
for the Pacific deep water above the sea-floor referred to above.

Three major points were made in the GEOSECS study regarding plutonium — and have
been confirmed in subsequent work:
(i) A strong subsurface maximum in Pu concentrations was observed over large areas
of the Pacific,
(ii) Significant increases in Pu concentrations were generally noted in deep water near
the sea-floor. (These increases seemed to be restricted to the western and northern
stations in the N Pacific region),
(iii) With the exception of the eastern GEOSECS stations between 30°-40°N, Pu
inventories in the water column substantially exceed those expected from global
fallout. Local fallout from Pacific nuclear weapons test sites is proposed as the
most likely explanation for this observation.

Figure 51 shows 239,240Pu profiles in water columns of the central NW Pacific Ocean at
GEOSECS, Hakuho Maru and IAEA stations (the positions of the sampling stations are
shown in Fig. 42). It is clear that after 24 years, the subsurface maximum became much

54
smaller and less pronounced (a decrease by about a factor of 4) and has moved to deeper
water layers (from 450 m to 850 m). Although the initial view of these changes (and as
discussed subsequently with respect to Pu inventory change over time) was that they were
caused by Pu association with sunken particle fluxes, this view almost certainly needs to be
revised in the light of new data for 90Sr and 137Cs. It has been shown that, in the upper 1000
m, the decline in 90Sr and 137Cs maxima and inventories is similar to the Pu changes. This
would lead to the conclusion that at least a major part of the observed Pu changes over time
was in response to physical circulation in the upper water column that brought advectively
into the region water masses bearing significantly lower levels of fallout nuclides.

A similar comparison in the development of the 239,240Pu profile in the water column can
be seen in Figs 52 and 53, where data from the GEOSECS, KNORR, and IAEA stations
situated west and east of Bikini Atoll, respectively, are compared. The vertical spread in the
Pu maxima is much smaller and the recent concentrations have been higher than in Fig. 51.
The concentrations and inventories at these stations did not change significantly over 24
years. As these stations are all in the westward flowing North Equatorial Current (with very
low biological productivity, oligotrophic conditions), the maintenance of the concentration
profiles and inventories in the upper ocean may be related to these water masses recirculating
in near-permanent low productivity conditions.

Although no difference is noted in Pu profiles in the upper ocean stations shown in

Figs 52 and 53, west and east of Bikini, substantial differences can be found in deep water
east of (upstream) and west of (downstream) the atolls. In Fig. 54, various Pu profiles east of
the islands are contrasted with others in between and west of the islands. A difference of
about a factor of two can be observed for deep-water Pu concentrations in the eastern (broken
lines) and western (solid lines) stations visited between 1973 and 1982. Higher deep-water Pu
levels were found in 1997 (IAEA station 6, northwest of Bikini). This east/west gradient may
have been created initially by the large test fallout patterns. A further explanation that may be
applicable could involve the continuous remobilization of Pu to deep water from heavily
contaminated material down the steep slopes from the atolls to the sea-floor. As deep-water
circulation is slow but heading to the northwest, elevated deep-water concentration levels to
the west of the islands could be maintained over time.

On the basis of all available 239,240Pu data in the central NW Pacific Ocean (between
20°–40°N and 135°–175°E), a time dependence of the position of the subsurface maximum in
the water column has been worked out. This linear dependence (on a semilogarithmic scale) is
shown in Fig. 55, documenting a similar trend at all sampling stations between 1973 and
1997. The 239,240Pu maximum moves downward in the water column reaching double the
depth in about 40 years. A decrease in the maximum 239,240Pu concentration observed at the
central NW Pacific stations with time is shown in Fig. 56. The change of the maximum
239,240
Pu concentration in the water column to a half value is reached after 22 ± 8 years. As
noted earlier, much of these observed changes may be physically driven.

As discussed, the input function by which Pu was introduced into the Pacific Ocean was
mainly two pulse injections into the surface layer in the early 1950s (local tropospheric
fallout) and in the early 1960s (global fallout). Therefore, Pu in the water column is in a
transient state and its concentrations and inventories should change with time according to
oceanographic, geochemical and biological processes that occur in the water column. Bowen
et al. [91] proposed that the 239,240Pu maximum they observed in the water column of the
Atlantic Ocean could be a result of the bacterial degradation of sinking particles with
subsequent release of plutonium.

55
 45
GEOSECS
[1973]
40 Knorr73
[1978]
KH-80-2
35 Stn-1 [1980]
GX-223
GX-224 KH-82-1
GX-225 [1982]
CY-11 Stn-3
North Latitude (deg.)

30
GX-226 IAEA 97
[1997]

25

20

St.14
15 Stn-8 St.4
St.13 St.3
St.6-St.8 St.2 CE-8
Enewetak Stn-6 GX-229
10 Bikini

130 135 140 145 150 155 160 165 170 175
East Longitude (deg.)

FIG. 42. GEOSECS (1973) [30], KNORR (1978) [82], Hakuho Maru (1980, 1982) [41, 80]
and IAEA (1997) [67] sampling stations in the NW Pacific Ocean (data used for the
evaluation of water profile time series).
90
S r (m B q /L )
0 1 2 3 4
0

1000

2000

G E O S E C S (1 9 7 3 )
Depth (m)

G X -2 2 3
3000 G X -2 2 4
G X -2 2 5
G X -2 2 6
K H -8 0 -2 (1 9 8 0 )

K H -8 0 -2 (1 9 8 0 )
4000 C Y -1 1
IA E A 9 7 (1 9 9 7 )

IA E A 9 7 (1 9 9 7 )
S tn - 1
S tn -3
5000
0
G E O S E C S :G X -2 2 3 -2 2 6
K H -8 0 -2 :C Y -1 1
IA E A 9 7 :S tn -1 + 3
6000

FIG. 43. 90Sr profiles in the water column of the GEOSECS (1973) [30], Hakuho Maru
(1980) [41] and IAEA (1997) [67] stations in the central NW Pacific Ocean.

56
 90
Sr (mBq/L)
0.0 0.5 1.0 1.5 2.0 2.5
0

500

1000

1500

2000
Depth (m)

2500

3000

Knorr73 (1978)
St. 7
3500 St. 8
IAEA97 (1997)

IAEA97 (1997)
4000 Stn-6
Series7
Knorr73:St. 7+8
IAEA 97:Stn-6
4500

FIG. 44. 90Sr profiles in the water column west of Bikini Atoll.
90
Sr (mBq/L)
0 1 2 3 4 5
0

1000

2000
Depth (m)

3000

4000

GEOSECS (1973)
GX-229
5000 Knorr73 (1978)

Knorr73 (1978)
St. 3
Series6

GEOSECS:GX-229
Knorr73:St. 3
6000

FIG. 45. 90Sr profiles in the water column east of Bikini Atoll.

57
 90
Sr (mBq/L)
0 1 2 3 4 5
0

1000

GEOSECS (1973)
GX-229
2000 Knorr73 (1978)

Knorr73 (1978)
St. 3
Depth (m)

St. 7

3000 St. 8
St. 14
KH-82-1 (1982)

KH-82-1 (1982)
CE-8
4000 IAEA97 (1997)

IAEA97 (1997)
Stn-6

GEOSECS:GX-229
5000
Knorr73:St. 3
Knorr73:St. 7+8+14
KH-82-1:CE-8
IAEA 97:Stn-6
6000

FIG. 46. A comparison of 90Sr profiles in the water column of stations east (broken lines) and
west (continuous lines) of Bikini Atoll).
137
C s (m B q /L )
0 1 2 3 4 5
0

1 0 00

G E O S E C S (1 9 7 3 )
2 0 00
G X -22 3
G X -22 4
G X -22 5
Depth (m)

3 0 00 G X -22 6
K H -8 0-2 (1 98 0)

K H -8 0 -2 (1 98 0 )
C Y -11

4 0 00 IA E A 97 (19 97 )

IA E A 9 7 (1 9 9 7 )
S tn - 1
S tn - 3
5 0 00
G E O S E C S :G X -2 2 3-2 2 6
K H -80 -2 :C Y -11
IA E A 97 :S tn -1
6 0 00

FIG. 47. 137Cs profiles in the water column of the GEOSECS (1973), Hakuho Maru (1980)
and IAEA (1997) stations in the central NW Pacific Ocean.

58
 137
Cs (mBq/L)
0 1 2 3 4 5
0

500

1000

1500

2000
Depth (m)

2500

3000
GEOSECS (1973)
St. 6
3500 St. 7
St. 8
IAEA97 (1997)

IAEA97 (1997)
4000 Stn-6
Series8

Knorr73:St. 6+7+8
IAEA 97:Stn-6
4500

FIG. 48. 137Cs profiles in the water column west of Bikini Atoll.
137
Cs (mBq/L)
0 1 2 3 4 5 6 7
0

1000

2000
Depth (m)

3000

4000

GEOSECS (1973)
GX-229
Knorr73 (1978)

Knorr73 (1978)
5000 St. 2
St. 3
St. 4

GEOSECS:GX-229
Knorr73:St. 2+3+4
6000

FIG. 49. 137Cs profiles in the water column east of Bikini Atoll.

59
 239+240
P u ( m B q /L )
0 0 .0 2 0 .0 4 0 .0 6 0 .0 8 0 .1
0

1000

2000

G E O S E C S (1 9 7 3 )
Depth (m)

G X -2 2 3
3000 G X -2 2 4
G X -2 2 5
G X -2 2 6
K H -8 0 -2 (1 9 8 0 )

K H -8 0 -2 (1 9 8 0 )
4000 C Y -1 1
IA E A 9 7 (1 9 9 7 )

IA E A 9 7 (1 9 9 7 )
S tn -1

5000 S tn -3
*D U M M Y

G E O S E C S :G X -2 2 3 -2 2 6
K H -8 0 -2 :C Y -1 1
IA E A 9 7 :S tn 1 + 3
6000

FIG. 50. A comparison of 137Cs profiles in the water column east (broken lines) and west
(continuous lines) of Bikini Atoll.

137
C s ( m B q /L )
0 1 2 3 4 5 6 7
0

1000

G E O S E C S (1 9 7 3 )
G X -2 2 9
K n o r r7 3 (1 9 7 8 )
2000
K n o rr7 3 (1 9 7 8 )
S t. 2
S t. 3
S t. 4
Depth (m)

S t. 6
3000 S t. 7
S t. 8
S t. 13
S t. 14
K H -8 2 - 1 (1 9 8 2 )

4000 K H -8 2 -1 (1 9 8 2 )
C E -8
IA E A 9 7 (1 9 9 7 )

IA E A 9 7 ( 1 9 9 7 )
S tn - 6

5000
G E O S E C S :G X -2 2 9
K n o rr7 3 :S t. 2 + 3 + 4
K n o rr7 3 :S t. 6 + 7 + 8 + 1 3 + 1 4
K H -8 2 -1 :C E -8
IA E A 9 7 :S tn -6
6000

FIG. 51. 239,240Pu profiles in the water column of the GEOSECS (1973), Hakuho Maru (1980)
and IAEA (1997) stations in the central NW Pacific Ocean.

60
 239+240
P u ( m B q /L )
0 0 .0 2 0 .0 4 0 .0 6 0 .0 8 0 .1
0

500

1000

1500

2000
Depth (m)

2500
K n o rr7 3 (1 9 7 8 )
S t. 6
3000 S t. 7
S t. 8
IA E A 9 7 (1 9 9 7 )

3500
IA E A 9 7 (1 9 9 7 )
S tn -6
G E O S E C S :G X -2 2 9
4000
K n o r r 7 3 : S t .6 + 7 + 8

IA E A 9 7 :S tn -6

4500

FIG.52. 239,240Pu profiles in the water column of the KNORR(1978) and IAEA (1997) stations
west of Bikini Atoll.

239+240
P u (m B q /L )
0 0 .0 2 0 .0 4 0 .0 6 0 .0 8 0 .1
0

1000

2000
Depth (m)

3000

G E O S E C S (1 9 7 3 )
G X -2 2 9
4000
K n o rr7 3 (1 9 7 8 )

K n o rr7 3 (1 9 7 8 )
S t. 2
S t. 3
5000 S t. 4
G E O S E C S :G X -2 2 9

G E O S E C S :G X -2 2 9

K n o rr7 3 :S t.2 + 3 + 4
6000

FIG. 53. 239,240Pu profiles in the water column of the GEOSECS (1973) and KNORR (1978)
stations east of Bikini Atoll.

61
 239+240
P u (m B q /L )
0 0 .0 2 0 .0 4 0 .0 6 0 .0 8 0 .1
0

1000

G E O S E C S (1 9 7 3 )
G X -2 2 9
K n o rr7 3 (1 9 7 8 )
2000
K n o rr7 3 (1 9 7 8 )
S t. 2
S t. 3
S t. 4
Depth (m)

S t. 6
3000 S t. 7
S t. 8
S t. 13
S t. 14
K H -8 2 -1 (1 9 8 2 )

4000 K H -8 2 -1 (1 9 8 2 )
C E -8
IA E A 9 7 (1 9 9 7 )

IA E A 9 7 (1 9 9 7 )
S tn -6
G E O S E C S :G X -2 2 9
5000 G E O S E C S :G X -2 2 9
K n o rr7 3 :S t.2 + 3 + 4
K n o rr7 3 :S t.6 + 7 + 8 + 1 3 + 1 4
K H -8 2 -1 :C E -8
IA E A 9 7 :S tn -6
6000

FIG. 54. A comparison of 239,240Pu profiles in the water column of the stations east (broken
lines) and west (continuous lines) of Bikini Atoll.

Recently, Hirose [49] developed a simple complexation-scavenging five-layer model to

explain vertical 239,240Pu profiles in the N Pacific Ocean. The transport rate constants for
dissolved plutonium (as in the case of trace metals) in sea water are expressed as the partition
coefficients of plutonium for particulate organic matter and Pu flux in sea water. The model
implies that the pattern of the 239,240Pu vertical profile is formed by the process of plutonium
being released in inorganic form, following the decomposition of sinking particles by
biogeochemical processes with depth. The model was tested using the results of sediment trap
experiments [92]. The plutonium residence times estimated by the model for 0–250 m and 0–
750 m depth layers are 10 and 33 years, respectively, in agreement with experimental
observations. The model has successfully reproduced the vertical 239,240Pu profiles in the water
columns as well. However, there are some limitations of the model in connection with
physical processes in the water column and chemical forms of plutonium. It has been shown
by Nelson et al. [64] (see also [93] for a later review) that the chemical form of plutonium
changes with water depth and this would imply that the plutonium partition coefficient will
not be constant through the water column either. There are still many uncertainties in Pu
aqueous chemistry and therefore, further work is required for a better understanding of
plutonium behaviour in the water column. In particular, the role of physical processes needs
to be defined.

Another typical feature of the 239,240Pu water profiles in the NW Pacific Ocean shown in
Figs 51 and 52 is an elevated 239,240Pu concentration (by about a factor of two) observed in
samples taken close to the sea-bottom. This feature has not been observed in water profiles

62
taken in the NE Pacific Ocean [30]. It has been shown by Buesseler [65] that higher
240
Pu/239Pu ratios associated with tropospheric fallout are found in deeper and bottom water
layers of the NW Pacific, as well as in surface sediment. This would indicate that the
tropospheric fallout from the Marshall Islands is more rapidly removed from surface water to
deeper water and to sediment, causing higher Pu concentrations and higher 240Pu/239Pu ratios
in NW Pacific bottom water and sediment.

FIG. 55. Movement of a subsurface 239,240Pu maximum in the water column with time (the
dotted lines show the 95% confidence interval).

FIG. 56. Dependence of 239,240Pu concentrations in the subsurface maximum with time.

63
4.6. Radionuclide inventories

4.6.1. Water inventories

The inventory of a radionuclide in a seawater column is calculated by interpolating its

concentration measured at each depth:
1 N 
I w =  (Wi +1 + Wi )(d i +1 − d i ) + 2 W1 d1 + 2 WN (d B - d N ) (1)
2  i =1 
where Iw is the radionuclide inventory in a seawater column (Bq/m2), N is the number of
sampling depths (the depth number is counted downward from the surface to the bottom), Wi
is the radionuclide concentration in sea water at depth I (Bq/m3), di is the i-th sampling depth
of sea water (m), and dB is the total depth to the bottom (m). When sea water at a sampling
station is collected at the surface, the second term of the right-hand side of the above equation
is not taken into account. If the total depth of a sampling station is not given, the third term is
also omitted.
90
Sr and 137Cs inventories in the water column were compared for GEOSECS and IAEA
stations (Figs 43 and 47). As expected, the 90Sr and 137Cs inventories decrease with time from
about 3.8 kBq/m2 to 1.4 kBq/m2 for 90Sr, and from about 5.5 kBq/m2 to 2.2 kBq/m2 for 137Cs.
A change of 239,240Pu inventories in the water column with time has been evaluated for
the central NW Pacific Ocean (between 20°–40°N and 135°–175°E) and the total water depth
between 5000 and 6000 m using data stored in the GLOMARD. The averaged data show that
the Pu inventory in water is slowly decreasing with time from about 130 Bq/m2 to 100 Bq/m2
(Fig. 57). The rate of decrease of the Pu inventory with time by a factor of two was estimated
to be about 50 years, but it is necessary to keep in mind the physical process changes
mentioned earlier.
It is clear that the inventories depend on the height of the water column and the
geographical position of the sampling station. As the 239,240Pu concentrations below 2000 m
are almost constant, to exclude dependence on water depth, the geographical distributions of
inventories were compared for 2300 m (the depth of the station east of Kamchatka). As shown
in Fig. 58, 239,240Pu water inventories normalized to the depth of 2300 m during the 1990s do
not show any latitudinal dependence; they are within the interval of 35–53 Bq/m2, but the data
density is very low. A higher inventory (74 Bq/m2) observed in the area of the Marshall
Islands is believed to be due to specific circulation processes as discussed earlier.
4.6.2. Sediment inventories

The input signal of 90Sr, 137Cs and 239,240Pu to NW Pacific Basin sediment should be
viewed over time-scales of decades only due to the short delivery time since the introduction
of anthropogenic radionuclides into the marine environment. Global fallout patterns show
maxima in 1963–1964 corresponding to the weapons testing in the early sixties. Thus,
anthropogenic radionuclide penetration due to sediment accumulation alone would be
confined to millimetres [83]. The observed penetration depths in the order of centimetres
imply that sediment accumulation is not important in governing radionuclide distribution. The
stratigraphic record of the upper decimetre of recently deposited deep-sea sediment may be
influenced by particle mixing by benthic fauna. Therefore, the depth distribution of
anthropogenic radionuclides in bottom sediment has to be interpreted with caution. On the
other hand, as sediment is the final depository of radionuclides in the sea, it provides
important information on scavenging processes in the water column, on deposition histories
of radionuclides and on accumulation processes occurring in sediments.

64
 FIG. 57. Changes in 239,240Pu inventories in the water column with time.

FIG. 58. 239,240Pu inventories (Bq/m2) in the water column (down to 2300 m) (the year of
sampling is shown in parentheses).

65
 90
Sr (Bq kg-1) 90
Sr (Bq kg-1)
0 2 4 6 8 10 0.0 0.4 0.8 1.2 1.6 2.0 2.4 2.8
0 0

1 1

Depth (cm)
2

Depth (cm)
3 3

4 4

5 5

-2 -2
St. 1 (Inventory 73 +/- 3 Bq m ) St. 8 (Inventory 19 +/- 5 Bq m )
90 -1
Sr (Bq kg )
0 1 2 3 4 5 6
0

Depth (cm)

-2
St. 9 (Inventory 11 +/- 5 Bq m )

FIG. 59. Depth distribution of 90Sr in bottom sediment of the NW Pacific Ocean (IAEA'97).

The data stored in the GLOMARD database show that radionuclide concentrations in
sediment cores (usually cores up to a depth of 15 cm were analysed) of the N Pacific Ocean
decrease with depth. Some of the undisturbed profiles however, have a peak at a few cm
below the surface. The surface radionuclide concentrations are higher in sediment collected in
the 1990s than in samples collected in the 1980s. The data show, however, a large variation in
radionuclide concentrations between sites.
The inventory of a radionuclide in a sediment core is estimated by summing its
concentration in each layer of sediment:
M
I s =  S i Di (U i - Li ) (2)
i =1
where Is is the radionuclide inventory in a sediment core (Bq/m2), M is the number of
sediment layers (the layer number is counted downward from the surface to the deeper layer),
Si is the radionuclide concentration in layer i (Bq/kg-dry), Di is the density of layer i (kg-
dry/m3), Ui is the upper boundary of layer i (m), and Li is the lower boundary of layer i (m).
90
4.6.2.1. Sr and 137Cs

Published sediment inventories have varied from 11 to 123 Bq/m2 for 90Sr and from 6.9
to 341 Bq/m2 for 137Cs in the NW Pacific Ocean, with low values near the Proving Grounds.
Similar values for inventories of 137Cs (4–111 Bq/m2) were reported earlier north of 30oN by
[38].
Sediment core samples were collected recently during the IAEA '97 NW Pacific Cruise
and the KORDI cruise to the West Caroline Basin [96] (Table X). Depth distributions and

66
inventories of anthropogenic radionuclide concentrations in bottom sediment from the NW
Pacific stations are presented in Figs 59 to 64, respectively.

The 90Sr concentrations in the top 0–0.5 cm surface sediment are 7.5 ± 0.8, 1.9 ± 0.3
and 2.8 ± 0.7 Bq/kg dw at IAEA stations 1, 8 and 9, respectively. Core top concentrations of
90
Sr show a latitudinal trend of increasing values away from the equator, that are similar to
137
Cs values in the region. Since 90Sr is more soluble in sea water than 137Cs, it participates in
the biological cycle through the formation of celestite (SrSO4) by acantharians as their
structural component [95].

137
Cs (Bq kg-1) 137
Cs (Bq kg-1)
0 5 10 15 20 25 30 35 40 0 1 2 3
0 0

2
1
3

4
2
Depth (cm)

Depth (cm)
5

3 7

9
4
10

11
5 12

St. 1 (Inventory 321 +/- 23 Bq m-2) St. 6 (Inventory 6.92 +/- 0.83 Bq m-2)

137
137
Cs (Bq kg-1) Cs (Bq kg-1)
0 1 2 3 4 5 6 0 1 2 3 4 5 6
0 0

1 1

2
Depth (cm)

2
Depth (cm)

3 3

4 4

5 5

St. 8 (Inventory 16 +/- 6 Bq m-2) St. 9 (Inventory 22 +/- 5 Bq m-2)

FIG. 60. Depth distribution of 137Cs in bottom sediment of the NW Pacific Ocean(IAEA '97).

The 90Sr distribution is more subject to regional biological influences than that of 137Cs. The
penetration depth of 90Sr is 3–4, 0.5–1.0 and 1–2 cm below the sea-floor at stations 1, 8 and 9,
respectively. The sediment inventory of 90Sr was estimated based on 90Sr concentration and
sediment mass accumulation per unit area and is 72 ± 3, 19 ± 5 and 11 ± 5 Bq/m2 at stations 1,
8 and 9, respectively.

67
 239,240
Pu (Bqkg-1) 239,240
Pu (Bqkg-1)
0.0 0.5 1.0 1.5 2.0 2.5 0 3 6 9 12 15 18
0 0

2 2

4 4

Depth (cm)

Depth (cm)
6 6

8 8

10 10

12 12

St. 1 (Inventory 28.6 +/- 0.4 Bq m-2) St. 6 (Inventory 132 +/- 3 Bq m-2)
239,240 239,240
Pu (Bqkg-1) Pu (Bqkg-1)
0 2 4 6 8 10 0.0 0.1 0.2 0.3 0.4
0 0

2
2

4
6
Depth (cm)

Depth (cm)

8 6

10
8

12

10
14

16 12

St. 8 (Inventory 72 +/- 1 Bq m-2) St. 9 (Inventory 2.8 +/- 0.2 Bq m-2)

239,240
FIG. 61. Depth distribution of Pu in bottom sediment of the Northwest Pacific Ocean
(IAEA'97).

TABLE X. LOCATION OF SEDIMENT SAMPLING STATIONS FROM THE NW

PACIFIC BASIN (IAEA) AND WEST CAROLINE BASIN (KORDI)
Station Sampling Latitude Longitude Water depth (m) Remarks
date
IAEA '97 Pacific Ocean Expedition
1 24 Oct ‘97 35o00.065N 145o59.569E 5924 Red clay
6 10 Nov ‘97 11o27.288N 164o52.413E 4537 Carbonate ooze
8 13 Nov ‘97 15o30.177N 159o30.536E 5390 Red clay
9 16 Nov ‘97 22o22.010N 152o40.584E 5600 Red clay
KORDI Cruise TOGA92
TEQ6 3 Dec ‘92 5o03.289N 137o01.277E 4629 Red clay
TEQ12 5 Dec ‘92 2o00.625N 137o00.036E 4157 Carbonate ooze

68
 90 90
Sr (Bq kg-1) Sr (Bq kg-1)

0 2 4 6 8 0 1 2 3 4 5 6
0 0

1 1

Depth (cm)

Depth (cm)
2 2

3 3

4 4

5 5

-2 -2
St. TEQ6 (Inventory 86 +/- 17 Bq m ) St. TEQ12 (Inventory 123 +/- 31 Bq m )

FIG. 62. Depth distribution of 90Sr in bottom sediment of the West Caroline Basin (TEQ9212,
1992).
137 137
Cs (Bq kg-1) Cs (Bq kg-1)

0 2 4 6 8 10 0 5 10 15 20 25
0 0

1 1
Depth (cm)

Depth (cm)

2 2

3 3

4 4

5 5

-2
St. TEQ6 (Inventory 249 +/- 44 Bq m ) St. TEQ12 (Inventory 371 +/- 81 Bq m-2)

FIG. 63. Depth distribution of 137Cs in bottom sediment of the West Caroline Basin TEQ9212,
1992).
239,240 239,240
Pu (Bqkg-1) Pu (Bqkg-1)

0.00 0.05 0.10 0.15 0.20 0.25 0.30 0.00 0.05 0.10 0.15 0.20 0.25 0.30
0 0

2 2
Depth (cm)

Depth (cm)

4 4

6 6

8 8
-2
St. TEQ6 (Inventory 6.82 +/- 0.51 Bq m ) St. TEQ12 (Inventory 8.95 +/- 0.62 Bq m-2)

239,240
FIG. 64. Depth distribution of Pu in bottom sediment of the West Caroline Basin
TEQ9212, 1992).

69
 In the West Caroline Basin, 90Sr concentrations in the top 0–0.5 cm surface sediment
are about 4.6 Bq/kg at stations TEQ6 and TEQ12. The penetration depth of 90Sr is 3–4 cm
below the sea-floor at stations TEQ6 and TEQ12. The sediment inventory of 90Sr was
estimated based on 90Sr concentrations and sediment mass accumulation per unit area and is
86 ± 17 and 123 ± 31 Bq/m2 at stations TEQ6 and TEQ12, respectively (Table XI).

TABLE XI. INVENTORIES OF ANTHROPOGENIC AND NATURAL RADIONUCLIDES

IN NW PACIFIC BASIN BOTTOM SEDIMENT (Bq/m2)
239,240 137 90
Station Pu Cs Sr
IAEA 1 28.6 ± 0.4 320 ± 20 73 ± 3
IAEA 6 132 ± 3 6.9 ± 0.8
IAEA 8 72 ± 1 16 ± 6 19 ± 5
IAEA 9 2.8 ± 0.2 22 ± 5 11 ± 5
KORDI 6 6.8 ± 0.5 250 ± 40 86 ± 17
KORDI 12 8.9 ± 0.6 370 ± 80 120 ± 30
137
Cs concentrations in the top 0–0.5 cm surface sediment are 27±3, 2.2±0.6, 3.4±1.7
and 4.3±1.6 Bq/kg dw at IAEA stations 1, 6, 8 and 9, respectively. Core top concentrations of
137
Cs show a latitudinal trend of increasing values away from the equator, which is the
opposite to 239,240Pu in the region. The higher 137Cs concentrations are generally confined to
the core top and decrease with depth at all stations. The penetration depth of 137Cs is 3–4, 7–8,
0.5–1.0 and 1–2 cm below the sea-floor at stations 1, 6, 8 and 9, respectively. The sediment
inventory of 137Cs was estimated based on 137Cs concentration and sediment mass
accumulation per unit area and is 320 ± 20, 6.9 ± 0.8, 16 ± 6 and 21 ± 5 Bq/m2 at stations 1, 6,
8 and 9, respectively. The activity ratio of 239,240Pu/137Cs in the core top sediment is 0.07, 5.7,
1.58 and 0.93 at stations 1, 6, 8 and 9. This pronounced latitudinal trend, also reported in
earlier studies [30, 83, 90] suggests that local fallout accounts for the high inventories of
239,240
Pu and that either less 137Cs was delivered in this fashion (due to its noble gas precursor)
or that more 137Cs was released from sinking particles. Nevertheless, the ratios of
239,240
Pu/137Cs at St. 6 still show higher values than the other stations. The direct effect of the
test sites decreases with latitude; surface circulation patterns may produce elevated ratios far
from the source. Also the interaction of Pu and Cs radionuclides with the sediment particles
are different. The distribution coefficient (Kd) is 104–105 for Pu and 102–103 for Cs [94].

In the West Caroline Basin, the 137Cs concentration in the top 0–0.5 cm surface
sediment is 10.7±3.6 and 16.6±5.5 Bq/kg dw at stations TEQ6 and TEQ12, respectively. The
penetration depth of 137Cs is about 3 cm below the sea-floor at both stations. The sediment
inventory of 137Cs is 250 ± 40 and 370 ± 80 Bq/m2 at stations TEQ6 and TEQ12, respectively
(Table XI).

4.6.2.2. Plutonium

The 239,240Pu inventories in sediment calculated for the N Pacific Ocean from
GLOMARD data are shown in Fig. 65. As expected, large variations are observed in 239,240Pu
inventories. The 239,240Pu inventory in sediment should grow slightly with time as more
plutonium is scavenged onto sediment from thewater column. However, it is difficult to
establish

70
 55
54
Knorr73 [1978]
50 43
6
KH-80-2 [1980]
45
MBC [1981, 82]
9
40 11 J-K-R Expedition
6 6
22 11 [1994, 95]
12
35 16 9
29 IAEA97 [1997]
7-52 2
30 8 MPG-1 Data from the GLOMARD
3 4 2-6 4
[1978-1996]
25 9 10
1
20
72
15

North Latitude (deg.)

35
132
Enewetak Bikini 2
10 880 260* 3
11 4
5 3
3
1
0 9

-5 1

1
-10
130 140 150 160 170 180 190 200 210 220 230 240 250 260 270
East Longitude (deg.)

FIG. 65. Sediment 239,240Pu inventories (Bq/m2). (*The inventory at Bikini Atoll was calculated for 0–4 cm depth only).

71
establish any time trend because the data are very sparse and large differences have been
observed even at stations in near proximity. The spatial distribution of Pu inventories suggests
that the inventories decrease from the region of the Marshall Islands to the central NW Pacific
(from about 100–900 to 10 Bq/m2), although the data density is very low. A decrease in
inventories is also observed from the region of the Marshall Islands to the equator [82]. There
is a clear indication that sediment inventories increase by a factor of three to five from the NE
to the NW Pacific Ocean, reflecting different Pu sources in the region (the data from the Mid-
Pacific gyre (MPG-1), KNORR, and other expeditions). This is in agreement with previous
observations [30, 65] that the NW Pacific Ocean is affected by tropospheric fallout from the
Marshall Islands area and its transport to the NW Pacific Ocean, while the NE Pacific Ocean
shows only global (stratospheric) fallout effects. Cochran [83], analysing data from the
MANOP sites (situated in the equatorial region east of the Christmas Islands) found
decreasing inventories northwards from the equator and with longitude east as well. This may
simply be the result of enhanced Pu removal in the higher-productivity waters centred on the
equator in the Eastern Pacific. When the MANOP sediment data are compared with the water
column inventory reported at the neighbouring GEOSECS station [30] this pattern fits well.
The reported inventory (59 Bq/m2) is nearly ten times that expected from global fallout. These
observations, plus the MANOP sediment data, plus their 240Pu/239Pu ratios (higher than
fallout) observed by Buesseler [65] seem consistent with a scenario whereby local fallout
from Enewetak and Bikini is transported eastwards to the eastern Equatorial N Pacific in the
strong N Equatorial Counter-Current and Pu is removed from the surface ocean in the flux of
sinking particles from the productive zone on the equator.

A more detailed study of Pu in sediment from IAEA stations shows that in the top 0–0.5
cm core section, 239,240Pu concentrations are 1.78±0.06, 12±1, 5.38±0.22 and 0.15±0.02 Bq/kg
dw at IAEA stations 1, 6, 8 and 9, respectively. Core top concentrations of 239,240Pu show a
latitudinal trend of decreasing values away from the equator, since atmospheric weapon test
sites are located on the equator (Enewetak and Bikini Atolls, 11oN, 162-165oE; Christmas
Island, 2o2’N 157o40’W; Mururoa and Fangataufa Atolls, 22oS, 140oW). 239,240Pu
concentrations decrease with depth at all stations (Fig. 61). 239,240Pu penetrated to the top
10 cm, top 6 cm, top 15 cm and top 7 cm below the sea-floor at stations 1, 6, 8 and 9,
respectively. However, subsurface maxima were observed at stations 1, 6 and 9. 238Pu
concentrations are 0.11±0.01, 0.43±0.10, 0.14±0.02 and 0.06±0.01 Bq/kg dw at stations 1, 6,
8 and 9, respectively. 238Pu was found in the top 4 cm below the sea-floor. The sediment
inventory of 239,240Pu was estimated based on the down core distribution of 239,240Pu
concentration and sediment mass accumulation per unit area and is 28.6 ± 0.4, 132 ± 3, 71.8 ±
0.9 and 2.8 ± 0.3 Bq/m2 at stations 1, 6, 8 and 9, respectively. The inventories at stations 1, 6
and 8 in the NW Pacific are much higher than those of the NE Pacific, but Station 9 shows
inventories similar to the NE Pacific [83]. The highest inventory found at St. 6 is due to local
fallout. Cochran [83] reported 239,240Pu concentrations in the core top 0–2 cm section as 0.3–
0.5 Bq/kg and its inventory is 2.67 to >8.50 Bq/m2 in the east Equatorial Pacific region
(140°W-90°W, 1-12°N). However, it is similar to those found in the deep basin of the Sea of
Japan [97] and in the NW Pacific off Kamchatka Peninsula [42, 44, 98]. The difference in
sedimentary 239,240Pu inventories between stations may be due to the latitudinal influence of
local fallout and/or sediment accumulation rates and surface water circulation. Activity ratios
of 238Pu/239,240Pu in bottom sediment varied from 0.01 to 0.06.
In the West Caroline Basin (2–5°N), in the top 0–0.5 cm core section, maximum
239,240
Pu concentrations are 0.08±0.01 and 0.10±0.01 Bq/kg dw at stations TEQ6 and TEQ12,
respectively. These values are much lower than the rest of the NW Pacific (IAEA '97),
probably due to the isolation of the basin by its high topographic relief. The West Caroline

72
Basin is approximately 4000 to 5000 m deep and is semi-enclosed with rises near Sonsorol
Island and the Caroline Islands as well as the Eauripik Rise in the east. These rises, which
separate the West Caroline Basin from the western N Pacific, are approximately 2000–
3000 m deep and allow Pacific deep water (approximately more than 2000 m depth) and
intermediate water (approximately 1000–2000 m depth) to enter the Basin. In the north, the
deep sill below approximately 4000 m is located along the Yap Mariana Trench (about 4000
to 8000 m deep), which connects the West Caroline Basin to the open western Pacific Ocean.
This strait serves as the only conduit for Pacific bottom water (approximately several
hundreds of metres above the sea-floor) to ventilate the West Caroline Basin [99]. Three
major currents are important in the West Caroline Basin: the North Equatorial Current and its
branch and the Equatorial Counter-Current. The North Equatorial Current is a westbound flow
and is observed between 25oN and 5oN near 170–180°E in February, while in August it
descends no lower than 10°N. On reaching the western end of the Pacific, the North
Equatorial Current comes up against the continental barrier of the Philippines, where it
divides into two branches. One branch turns to the south and feeds the eastbound Equatorial
Counter-Current [100]. Depth distribution of 239,240Pu concentrations shows subsurface
maxima at 3–4 cm and 2–3 cm below the sea-floor. The sediment inventory of 239,240Pu was
estimated based on 239,240Pu concentrations and sediment mass accumulation per unit area and
is 6.82 ± 0.51 and 8.95 ± 0.62 Bq/m2 at TEQ 6 and TEQ 12, respectively. 238Pu concentrations
are equal to or less than the analytical detection limit of 0.01 Bq/kg at both stations.

In order to facilitate comparison of the 239,240Pu load at a given site with the different
sources of input, the total 239,240Pu inventories have to be calculated, i.e. the sum of the water
column and sediment inventories. The 239,240Pu water inventories constitute the greater part of
the total inventories, the contributions usually being around 90% except for the station east of
Kamchatka, where due to intense biological activity and high scavenging rates, the sediment
contribution has reached 50% of the total inventory.
Compared to the estimated global fallout deposition densities [101] the observed total
239,240
Pu inventories in the central NW Pacific Ocean show a surplus of about 100%. Of
course, after three decades of plutonium input from atmospheric nuclear bomb tests, the
geographical distribution of plutonium in the oceans will not be at steady state condition, but
will be affected by a complex of processes occurring in the marine environment. Horizontal
advection, upwelling and downwelling of water masses and biogeochemical processes in the
water column have played an important role in the development of the present distribution of
plutonium in the ocean. A plausible explanation for the surplus, which is consistent with
previous observations [30, 40, 42, 63, 65] may be the additional input from local fallout
transported from the tropics to the N Pacific Ocean.

4.7. Radionuclides in the Far Eastern Seas

4.7.1. Sea of Japan

4.7.1.1. Surface water time series

Levels of anthropogenic radionuclides (90Sr, 137Cs and 239,240Pu) in surface water of the
Sea of Japan (Box 14) are evaluated based on the HAM database. The total number of 137Cs,
90
Sr and 239,240Pu concentrations in the HAM database are 445, 593 and 126, respectively.
Some additional data have been added from the GLOMARD database.

Maps showing the sampling stations for surface water in the Sea of Japan for the period
1991–1995 and 1996–2000 are shown in Figs 66–68.

73
 Time series of 90Sr, 137Cs and 239,240Pu during 1971–1998 are examined to estimate their
concentrations in 2000. For 90Sr and 137Cs surface concentrations decrease exponentially,
whereas surface 239,240Pu concentrations show a slight change over the past two decades
(Fig. 69). The surface concentrations of 137Cs and 90Sr in the Sea of Japan in 2000 are
estimated to be 2.5 mBq/L and 1.4 mBq/L from the corresponding regression lines,
respectively. The surface concentration of 90Sr in the Sea of Japan in 2000 is similar to the
level in the western N Pacific (Box 4). The surface 239,240Pu concentration in the Sea of Japan
in 2000 is calculated to be 5.2 μBq/L, more than double the highest value estimated for each
box in the Pacific. The higher concentration of surface 239,240Pu is explained by rapid cycling
of 239,240Pu between the surface and subsurface layers, which is consistent with a small change
in surface 239,240Pu concentration [102].

The effective half-lives of 137Cs and 90Sr in surface water of the Sea of Japan are 19
and 14 years, respectively. The effective half-lives of 137Cs and 90Sr are similar to the mid-
latitude region of the western N Pacific (Box 4). The result could imply that surface 137Cs and
90
Sr in the Sea of Japan are controlled by the Tsushima Current, a branch of Kuroshio
Current. The effective half-life of 239,240Pu was estimated to be 16 ± 3 years, which seems to
be too long in comparison with Box 4 (7 ± 1 year).

4.7.1.2. Vertical profiles

The vertical profiles of 90Sr, 137Cs and 239,240Pu in the Sea of Japan (the locations are
given in Fig. 70) are shown in Figs 71–73. The 90Sr and 137Cs concentrations in the water
column decrease exponentially with increasing depth [45, 103]. However, the gradient of the
decrease rate with depth is smaller than that of the western N Pacific [104]. Especially the
vertical profile of 137Cs in the central northern region of the Sea of Japan [50] indicates that
relatively high values were observed in the deep layer. This can be explained by physical
processes such as vertical mixing in winter [105].
90
Sr and 137Cs vertical profiles, which are mainly controlled by physical processes,
indicate the penetration of these radionuclides into deep water as well. All these observations
suggest that a large part of anthropogenic radionuclides is stored in deep water as vertical
mixing in the Sea of Japan is more rapid than in the NW Pacific Ocean.
The vertical profile of 239,240Pu in the Sea of Japan (Fig. 73) shows a surface minimum,
subsurface maximum and decreases with increasing depth. Similar vertical profiles of 239,240Pu
were observed in the western N Pacific [30, 42, 67] and the Mediterranean [106]. However,
the pattern of the vertical 239,240Pu profile in the Sea of Japan is rather broad compared with
that in the western N Pacific [102, 103,] which is consistent with the result obtained in the
central north Sea of Japan [50]. This observation can be explained by the rapid recycling of
plutonium between the surface and subsurface layers due to winter convection.

The higher surface 239,240Pu concentrations found in the Sea of Japan in comparison with
the NW Pacific Ocean (Fig. 51) could be explained by winter upwelling of medium-deep
(below 500 m) Pu-enriched water [50]. The higher 239,240Pu concentrations at the surface, a
rather broad 239,240Pu maximum and higher concentrations observed in deep water suggest
recycling on a shorter time-scale than in the NW Pacific.

74
 48 48

46 46

44 44

r 42 42
(

north
north
40 40
i i

North Latitude

North Latitude
Latitude
Latitude
38 38

36 36

34 34

32 32

128 130 132 134 136 138 140 142 128 130 132 134 136 138 140 142
East Longitude East Longitude
FIG. 66. 90Sr sampling stations in the Japan Sea for the period 1991-1995 (left) and 1996-2000 (right).

75
 For the 239,240Pu inventory in water, a value of 0.12 kBq/m2 has been obtained, which is
higher by about a factor of 2 than expected from global fallout. This estimation is consistent
with previous data discussed earlier, explaining the additional input from local fallout
transported from the tropics to the N Pacific Ocean and specific oceanographic conditions in
the Sea of Japan [50].

4.7.1.3. Sediment

The results for 90Sr show very low concentrations, as expected, because only a small
fraction of the 90Sr input will settle with sinking particulates. The 137Cs/90Sr activity ratios are
generally higher than the global fallout ratio.
239,240
Pu concentrations in sediment differ significantly between sampling sites (as do
concentrations of 137Cs), the main reason being the higher removal rates in shallow water.
Generally, 239,240Pu concentrations in sediment at shallower water depths show higher values,
as expected. 238Pu/239,240Pu activity ratios were the same as the global fallout ratio. The
observed inventories are in the range 0.01–0.06 kBq/m2 for 90Sr, 0.05–0.4 kBq/m2 for 137Cs
and 0.001–0.12 kBq/m2 for 239,240Pu. The variation in the total water and sediment inventories
between sampling sites is very small.

4.7.2. The Sea of Okhotsk

90
Sr, 137Cs and 239,240Pu concentrations in surface and bottom water show variations
between the sampling stations depending primarily on the thickness of the water column. No
vertical distributions were available for comparison with the Sea of Japan and/or NW Pacific
data. Higher concentrations observed in bottom water could be explained by the high removal
rates in productive shallow water. The 238Pu/239,240Pu activity ratios did not differ statistically
from the values expected from global fallout. Similar conclusions could be drawn for 239,240Pu
concentrations in sediment. The data for shallow stations in the Sea of Okhotsk show
significantly higher sediment inventories than in the Sea of Japan or the NW Pacific.
However, the total inventories (water and sediment) did not differ considerably.

4.7.3. The Yellow and East China Seas

The Yellow Sea is a semi-enclosed continental shelf with a surface area of 380 x 109 m2
and an average depth of 44 m, and is surrounded by the contiguous land mass of China and
the Korean Peninsula.

In surface water, dissolved 90Sr concentrations varied from 1.97 to 2.58 mBq/kg with a
mean value of 2.34 ± 0.08 mBq/kg, generally lower in the coastal area than the open sea, and
high values were observed in Kyonggi Bay, where the Han River discharges. 137Cs
concentrations varied from 1.78 to 3.38 mBq/kg with a mean value of 2.63 ± 0. 21 mBq/kg.
The 239,240Pu concentrations varied from 2.17 to 13.35 Bq/kg with an average concentration
of 6.11 ± 0.32 Bq/kg for 1999 [107].
In bottom sediment, 90Sr concentrations varied from 0.6 to 3.9 Bq/kg with an average of
2.4 ± 1.8 Bq/kg in the upper 2 cm layer. 137Cs concentrations varied from 0.1 to 11.2 Bq/kg in
the upper 1 cm layer of bottom sediment. 239,240Pu concentrations varied from 0.1 to 0.9 Bq/kg
in the upper 1 cm layer. 137Cs and 239,240Pu radionuclides are heavily enriched in the finer
fraction of the sediment particle size [107].

76
 48 48

46 46

44 44

42 42

(degree)

(degree)
40 40

North Latitude

North Latitude
38 38

North Latituce

North Latituce
36 36

34 34

32 32

128 130 132 134 136 138 140 142 128 130 132 134 136 138 140 142
East Longitude (dgree) East Longitude (dgree)
FIG. 67. 137Cs sampling stations in the Japan Sea for the period 1991-1995 (left) and 1996-2000 (right).

77
78
48 48

46 46

44 44

42 42

(degree)

(degree)
Latitude
40

Latitude
40

Latituce

Latituce
North

North
38 38

North

North
36 36

34 34

32 32

128 130 132 134 136 138 140 142 128 130 132 134 136 138 140 142
East Longitude (dgree) East Longitude (dgree)

FIG. 68. 239,240Pu sampling stations in the Japan Sea for the period 1991-1995 (left) and 1996-2000 (right).
 Box14
100

Sr (mBq/L)
10
90

0.1
1950 1960 1970 1980 1990 2000
Year

Box 14
100
Cs (mBq/L)

10
137

0.1
1950 1960 1970 1980 1990 2000
Year

Box 14
100

10
Pu (µBq/L)

1
239+240

0.1

0.01
1950 1960 1970 1980 1990 2000
Year

FIG. 69. 90Sr, 137Cs and 239,240Pu time series in surface water of the Sea of Japan.

79
 55
No.3
No.7, 8
BG1 R4
R2 No.4
R3
50 R1
BG2 R5

Russia
N o rth la titu d e

45
No.5,N7 Vladivostok Otaru
No.6,N6 No.1,9
N1,2,3 Kushiro
5,4
BG1
40 1st expedition
1st expedition
Tonghae No.2,10
2nd expedition
K1 BG2 2nd expedition
Niigata
Korea Japan Dumping area
BG4 Dumping area
35 BG3
J1 Sampling
Sampling station
station
J2
J3 Background
Background station

30
125 130 135 140 145 150 155 160 165
East longitude
FIG. 70. Sampling stations in the Sea of Japan.

90
Sr (mBq/L)
0 2 4 6 8 10
0

500

1000

1500
Depth (m)

2000

2500
1964
1977
3000 1993
1994
1995
3500 1996
1997
N2 (1994)
4000

FIG. 71. 90Sr vertical profiles in the Sea of Japan.

80
 137
Cs (mBq/L)
0 5 10 15
0

500

1000

1500
Depth (m)

2000

2500

1964
3000 1977
1993
1994
1995
3500
1996
1997
N2 (1994)
4000

FIG. 72. 137Cs vertical profiles in the Sea of Japan.

239+240
Pu (µBq/L)
0 20 40 60
0

500

1000

1500
Depth (m)

2000

2500

1984
1993
3000 1994
1995
1996
1997
3500 N2 (1994)
1977(avg)

4000

FIG. 73. 239,240Pu vertical profiles in the Sea of Japan.

81
 Unfiltered surface water in the East China Sea contained 2.5–3.0 mBq/kg 137Cs, 1.9–2.8
mBq/kg 90Sr and 3.8–6.3 Bq/kg 239,240Pu in 1994 [107].

5. INDIAN AND SOUTHERN OCEANS

The Indian Ocean differs from the Atlantic and Pacific Oceans in its limited northward
extent, to only 25°N. The southern boundary of the ocean is usually taken at the Subtropical
Convergence at about 40°S. Its equatorial current system (Fig. 14) is strongly influenced by
the seasonal variation in the winds north of the equator. From November to March these
winds blow from the northeast (North East Monsoon), while from May to September they
blow from the southwest (South West Monsoon). The South West Monsoon is a continuation
across the equator of the South East Trade Winds that continue throughout the year. The
change of wind direction north of the equator then results in a change of currents there.
During the North East Monsoon season the North Equatorial Current (NEC) flows westward
from 8°N to the equator; the Equatorial Counter-Current (ECC) flows eastward from the
equator to 8°S and the South Equatorial Current (SEC) flows westward from 8°S to 15-20°S.
During the South West Monsoon the flow north of the equator is reversed. This combines
with the eastward ECC and the whole eastward flow from 15°N to 7°S becomes the Monsoon
Current. The SEC continues to the west, south of 7°S but is stronger than during the North
East Monsoon season.

During the North East Monsoon season, the SEC, when reaching the African coast,
supplies both the ECC to its north and the Agulhas Current flowing south, close to the African
shore. When it reaches the southern tip of Africa, the Current turns east into the Circumpolar
Current. During the South West Monsoon, the part of the SEC turning north supplies the
Somali Current up to the east coast of Africa. The SEC, the Somali Current and the Monsoon
Current then comprise a strong wind-driven gyre in the Northern Indian Ocean. Strong
upwelling occurs at this time along the Somali and Arabian coasts.

Along the eastern boundary of the Indian Ocean, off Western Australia, the Leeuwin
Current flows poleward along the continental shelf break from about 22°S to 35°S. The
Current then turns eastward. The Leeuwin Current is warm and of relatively low salinity, low
dissolved oxygen and high phosphate content, and transports a significant amount of heat to
the south.

Complex interaction between water masses takes place at frontal regions in the Southern
Ocean (south of 40°S). Antarctic bottom water (AABW) has been shown to spread throughout
the Southern and Northern hemispheres at 3000 to 4000 m water depth at frontal areas in mid-
latitudes. Because of these oceanographic parameters, mid-latitudes in the Southern Ocean are
high-nutrient low-chlorophyll zones (HNLC). The Southern Ocean region has also been
documented as a major sink of CO2 and is thus a highly productive area.

5.1. Radionuclides in surface water

Very few data have been reported to date on anthropogenic radionuclide concentrations
in the Indian Ocean. The only comprehensive study was carried out in 1978 in the framework
of the GEOSECS programme and included several vertical profiles of tritium in the water
column [108].

There was a latitudinal trend of tritium concentrations, but, already in 1978, it did not
reflect the fallout deposition in the area, but was influenced by water mass transport. Low

82
levels characterized the area below 40°S, while the highest concentrations were found
between 30°S and 10°S. Towards the north, tritium concentration regularly decreased around
the equator, to 10°N and levelled in the Arabian and Red Seas.

A few other data were obtained in [46] in the 1980s (137Cs from 2.8 to 2.9 Bq/m3) and in
[56] in 1994 when 137Cs concentrations ranged between 1.6 and 2.3 Bq/m3, while 90Sr ranged
from 1.1 to 1.5 Bq/m3. Only 3 results were reported for plutonium isotopes. Again, the lowest
levels characterized the area below 30°S.

The Indian Ocean together with the Southern Ocean was divided into 4 boxes (Fig. 15).
Data for 3H, 90Sr, 137Cs and 239,240Pu for the years 1991–1995 and 1996–2000 are plotted in
Figs 74 to 77. There were only a few data for the first time interval, therefore a proper
evaluation was not possible. For the second time period, thanks to the WOMARS project,
more data have become available from cruises to the Arabian Sea, the Southern Ocean and the
Indian Ocean transect. All investigated radionuclides show similar latitudinal trends with the
smallest values in Box 13 (below 60°S) and the highest in the centre box between 10°S and
35°S (Box 16, Tables VI–VIII). The broken latitudinal dependence in radionuclide
concentrations in surface water must be due to specific circulation patterns in the Indian
Ocean.

In the framework of the WOMARS project, a sampling campaign was carried out in
March–April 1998, along a track from New Zealand to the Mediterranean Sea (Fig. 78), to
determine the present concentrations of anthropogenic radionuclides in surface water. The
results for 3H, 90Sr, 137Cs and 239,240Pu are shown in Figs 79–82 as a function of latitude. The
latitudinal trend of radionuclide concentrations shows exactly the same trend as that of
GEOSECS tritium: low concentrations of both 137Cs and 90Sr (1.1–1.8 Bq/m3 and 0.7–1
Bq/m3, respectively) characterize the Tasman Sea and the whole area south of Australia, at
latitudes ranging between 40°S and 35°S. Proceeding northwest, all other stations in Box 16
show higher concentrations of both radionuclides (2.08–2.23 Bq/m3 for 137Cs and 0.76–1.5
Bq/m3 for 90Sr). Upwelling near the equator is probably responsible for the decrease in
concentrations in the latitudinal band 10°S and 10°N.

The Arabian and Red Seas are characterized by similar radionuclide concentrations, in
the range of 1.4–1.7 Bq/m3 for 137Cs and 0.9–1.4 for 90Sr. The mean ratio 137Cs/90Sr is 1.63 ±
0.19 (Fig. 83).
3
H data (Fig. 79) show the same latitudinal trend as the other radionuclides. The region
south of Australia and the Arabian Sea have lower concentrations than other areas. The
137
Cs/3H ratio is 0.019 ± 0.004 and the correlation coefficient is 0.74 ± 0.09 (Fig. 84). 239,240Pu
data in Fig. 82 show a similar latitudinal dependence to the other radionuclides.

83
 30
H (1996-2000)
3

20 Unit: mBq/L

10
150±70
(18)
0 150 ± 70
(18)
-10
Latitude

-20 170 ± 50
(5)
-30
-40 80 ± 60
(8)
-50
-60
-70
-80
20 40 60 80 100 120 140 160 180
Longitude

FIG. 74. 3H in the Indian and Southern Oceans (no data for 1991–1995) (data corrected to
01.01.2000).

5.2. Surface water radionuclide time series

Surface water 90Sr, 137Cs and 239,240Pu concentration time series for boxes 15, 16 and 17
(Fig. 15) were evaluated using data stored in the GLOMARD database. Figs 85–87 show the
data used for evaluation. The estimated effective half-lives of 90Sr, 137Cs and 239,240Pu in
surface water for different latitudinal boxes are given in Tables VI–VIII. 90Sr data were very
sparse so any estimation of effective half-lives was not possible. The concentrations for the
year 2000 were estimated from the few recent measurements available. 137Cs data enabled to
calculate the effective half-life which is around 20 years. The uncertainty in 239,240Pu data was
too high, except for Box 17 which gave an effective half-life of about 9 years.
137 239,240
When the data are grouped (Table XII), the effective half-lives for Cs and Pu
are 20 ± 2 years and 9 ± 2 years, respectively.

5.3. Radionuclides in the water column

GEOSECS Stations 413 (13°21'N; 53°13'E), 416 (19°45'N; 64°37'E) and 417 (3°57'N;
56°30'E) in the Arabian Sea (Fig. 88) were re-visited in 1998 to sample large volumes of
water at different depths. While Station 413, east of the Gulf of Aden, is relatively shallow
(bottom depth 2830 m), Station 416 in the north was 3210 m deep and Station 417 was the
deepest (4114 m). 137Cs data are presented in Figs 89–91. As there are no water profile data
for 137Cs from GEOSECS or other cruises, no direct comparison can be made for the Indian
Ocean. However, it is possible to compare the 137Cs profiles calculated from the measured
GEOSECS 3H profiles using the estimated 137Cs/3H ratio, as shown in Figs 89–91.

84
 30
90Sr (1991 -1995)
20
Unit: mBq/L
10

-10
e
Latitude

d 1.27 ± 0.01
u -20
itt (2)
-30

-40 0.5 ± 0.6

(2)
-50
-60
0.1 ± 0.1 (1)
-70

-80
20 40 60 80 100 120 140 160 180
Longitude

30 90Sr (1996 -2000)

20 Unit: mBq/L

10
1.0 ± 0.2
0
(15)
-10
Latitude

e
d
u -20 1.1 ± 0.2
tti
a (7)
L -30

-40
0.7 ± 0.4
-50 (12)

-60

-70

-80
20 40 60 80 100 120 140 160 180
Longitude

FIG. 75. 90Sr in the Indian and Southern Oceans (data corrected to 01.01.2000).

85
 30
137 Cs (1991-1995)
20 Unit: mBq/L

10

-10
Latitude

1.9 ± 0.2
-20
(2)
-30

-40
0.8 ± 0.9
-50
(2)
-60
0.1 ± 0.1 (1)
-70

-80
20 40 60 80 100 120 140 160 180
Longitude

30
137Cs (1996-2000)
20 Unit: mBq/L

10

0 1.6 ± 0.3
(17)
-10
Latitude

-20
2.1 ± 0.3
-30 (7)

-40
1.0 ± 0.6
-50
(12)
-60

-70

-80
20 40 60 80 100 120 140 160 180
Longitude

FIG. 76. 137Cs in the Indian and Southern Oceans (data corrected to 01.01.2000).

86
 30
239,240 Pu (1991-1995)
20 Unit: ųBqL

10

-10
Latitude

-20

-30

-40 1.4 ± 0.5

-50 (2)

-60

-70

-80
20 40 60 80 100 120 140 160 180
Longitude

30
Pu (1996-2000)
239,240

20 Unit: ųBq/L

10

0 1.9 ± 1.2
(13)
-10
Latitude

-20 3.0 ± 1.5

(4)
-30

-40
1.0 ± 0.4
-50 (10)

-60

-70

-80
20 40 60 80 100 120 140 160 180
Longitude

FIG. 77. 239,240Pu in the Indian and Southern Oceans.

87
 41

88
40
40 39
38
37
36
35
34
30
33
32
20
31
3029 28
27
10
26
25
24
0 23
22
21
20
-10 19
18
17

North Latitude (degree)

-20 16
15
14
-30 13
12 11
10 9 8 7 65 4 3 2
-40 1

10 20 30 40 50 60 70 80 90 100 110 120 130 140 150 160 170 180

Longitude (degree)

FIG. 78. Sampling stations of the Indian Ocean Transect Cruise, 1997.
 2.5

3H (TU), 1998 Cruise

3H (TU), GEOSECS (decay corrected)
2.0
H (TU)

1.5
3

1.0

0.5

0.0
-40 -20 0 20 40
3
FIG. 79. H concentrations in surface water of the Indian Ocean, the Red and Mediterranean
Latitude
Seas as a function of latitude.

2
Sr (Bq.m )
-3
90

0
-40 -20 0 20 40
Latitude

FIG. 80. 90Sr concentrations in surface water of the Pacific and Indian Oceans, the Red and
Mediterranean Seas as a function of latitude.

89
 4

Cs (Bq.m ) 3
-3

2
137

0
-40 -20 0 20 40
Latitude

FIG. 81. 137Cs concentrations in surface water of the Pacific and Indian Oceans, the Red and
Mediterranean Seas as a function of latitude.

Pu-239+240

6
Pu (mBq. m-3)

4
239,240

0
-40 -20 0 20 40
Latitude

FIG. 82. 239,240Pu concentrations in surface water of the Pacific and Indian Oceans, the Red and
Mediterranean Seas as a function of latitude.

90
 3

Sr-90 (Bq m )
-3
2

0
0 1 2 3
-3
C s-1 3 7 (B q m )

FIG. 83. Relationship between 137Cs and 90Sr in surface seawater.

3
H-3 (TU)

0
0 1 2 3 4
-3
C s -1 3 7 ( B q m )

FIG. 84. Relationship between 137Cs and 3H in surface seawater.

91
 FIG. 85. 90Sr time series in Indian Ocean surface water.

92
FIG. 86. 137Cs time series in Indian Ocean surface water.

93
 FIG. 87. 239,240Pu time series in Indian Ocean surface water.

94
 30

25

20

GX 416

15
GX 413
GX 417

10
GX 418

GX 419

50 55 60 65 70 75
FIG. 88. GEOSECS stations in the Arabian Sea revisited in 1998.

TABLE XII. MEAN EFFECTIVE HALF-LIVES OF 137Cs AND 239,240Pu IN INDIAN

OCEAN SURFACE WATER
Effective half-life ± 1σ*
(year)
Area Boxes 137 239,240
Cs Pu

North Indian Ocean 15 20.2 ± 1.9 21.2 ± 7.6

South Indian Ocean 16+17 21.9 ± 6.3 8.8 ± 1.0
All Indian Ocean 15-17 20.3 ± 1.8 9.0 ± 1.7
* Error weighted averaged values

95
 137
C s (m B q /L )
0 0 .5 1 1 .5 2
0

500

Depth (m) 1000

1500

2000

2500 G X -4 1 3
[1 9 7 8 ]
A S -0 3
[1 9 9 8 ]
3000

FIG. 89. Comparison of measured (dotted line) and calculated (continuous line), using
GEOSECS 3H data, 137Cs profiles at GEOSECS Station 413.

137
C s (m B q /L )
0 0 .5 1 1 .5 2
0

500

1000
Depth (m)

1500

2000

2500 G X -4 1 6
[1 9 7 8 ]
A S -0 1
[1 9 9 8 ]
3000

FIG. 90. Comparison of measured (dotted line) and calculated, (continuous line) using
GEOSECS 3H data, 137Cs profiles at GEOSECS Station 416.

96
 137
C s (m B q /L )
0 0 .5 1 1 .5 2
0

500

1000
Depth (m)

1500

2000

2500 G X -4 1 7
[1 9 7 8 ]
A S -0 4
[1 9 9 8 ]
3000

FIG. 91. Comparison of measured (dotted line) and calculated (continuous line), using
GEOSECS 3H data, 137Cs profiles at GEOSECS Station 417.

6. ATLANTIC AND ARCTIC OCEANS

The radioactive contamination of the Atlantic and Arctic Oceans originates from three
main sources:

• Global fallout, due to nuclear weapons testing in the atmosphere, which

occurred from 1945 to 1980,
• Nuclear reprocessing in western Europe notably Sellafield in the UK and Cap de
la Hague in France. The maximum discharges to the sea took place from 1970 to
1985,
• The Chernobyl accident in the Ukraine in 1986.

In contrast to the Pacific Ocean, the Atlantic has not received local fallout from nuclear
weapons testing to any significant extent. Due to the inputs from reprocessing and Chernobyl,
the NE Atlantic shows higher concentrations of, in particular, 137Cs, 99Tc and 129I than any
other part of the world ocean. Furthermore the variation in radionuclide concentrations is
higher than seen elsewhere. The marginal seas of Europe show concentrations of e.g. 137Cs
and 99Tc, which vary orders of magnitude within distances of a few hundred kilometres. It
thus is difficult to give meaningful average concentrations for these radionuclides in marginal
seas such as the North Sea, the Baltic Sea, the Black Sea and especially, the Irish Sea.

Intensive sampling of the NE Atlantic, including deep-water samples, was carried out in
the area of the NEA/OECD dumpsites for low level radioactive wastes by the Bundesamt für

97
Seeschiffahrt und Hydrographie (BSH) (Germany) between 1983 and 1985 [109]. The levels
detected are a consequence of global fallout from atmospheric weapons tests in the sixties.
137
Cs levels were between 2.8 and 4.5 Bq/m3 with an average concentration around 3.3 Bq/m3.
The 90Sr concentration was found to have an almost linear relation to 137Cs values with the
137
Cs/90Sr ratios close to the theoretical value of about 1.5 given in the UNSCEAR Report
[110]. 239,240Pu values were found to be relatively homogeneously distributed in the water
column between 5 and 30 mBq/m3, whereas maximum values were found at about 1000 m
depth. These observations were found to be similar to other oceans.

In order to collect more recent data on the background radionuclide levels in Atlantic
water flushing through the North Sea, a cruise on board the German R/V "Deneb" was carried
out in the spring of 1997 to the Mediterranean (Monaco). Samples of water taken at depths
down to 500 m were analysed for 137Cs, 90Sr and transuranics. The average levels found in
surface water of the eastern Atlantic and the Mediterranean are not statistically
distinguishable (Table XIII).

TABLE XIII. AVERAGE 90Sr AND 137Cs LEVELS IN 1997 IN ATLANTIC AND
MEDITERRANEAN SURFACE WATER (Bq/m3)
137 90
Cs Sr
Atlantic Ocean 2.33 ± 0.21 (24 values) 1.53 ± 0.21 (24 values)
Mediterranean Sea 2.63 ± 0.42 (25 values) 1.77 ± 0.31 (24 values)

The activity ratios of 137Cs/90Sr were 1.52 and 1.48, close to the expected fallout value.
The distribution of transuranics in surface water of the Atlantic is less homogeneous. For
239,240
Pu values were between 2.7 and 8.9 mBq/m3, while concentrations in deeper water
increased up to 17 mBq/m3. The activity ratios of 238Pu/239,240Pu are about 0.1, indicating
slightly higher ratios than expected from global fallout. The few data for the French
Mediterranean coast are above levels for the Atlantic, between 9.3 and 16.9 mBq/m3 for
239,240
Pu. Water from 500 m depth with levels up to 28 mBq/m3 of 239,240Pu possibly indicate
the influence of the nuclear complex at Marcoule on the Rhone river. The concentrations of
241
Am are mostly below 3 mBq/m3 down to 500 m depth and there is no obvious difference
between the data from the Atlantic and Mediterranean.

6.1. Surface water radionuclide time series in the Atlantic Ocean

The Atlantic and Arctic Oceans with their marginal seas have been divided into Boxes
18–30 (Fig. 92). The maps of the distributions and average concentrations for 3H, 90Sr, 137Cs
and 239,240Pu in Atlantic surface water for the period 1991–1995 and 1996–2000 are shown in
Figs 93 to 96 and 97 to 100, respectively. Unfortunately, for the south Atlantic Ocean, the
radionuclide data are very sparse, therefore a proper evaluation has not been possible.
Data for 137Cs for the period 1991–1995 clearly show a latitudinal effect with mean
concentrations from the south of 0.6 Bq/m3 (Box 30) to 3.5 Bq/m3 in the north (Box 18). The
highest concentrations were however, observed in the Baltic Sea (mean value of about 60
Bq/m3) and the Black Sea (about 40 Bq/m3). The data for the period 1996–2000 (where
available) show a similar trend.
The latitudinal effect is clearly seen for 90Sr as well. Higher mean concentrations were
observed in the Baltic Sea (about 10 Bq/m3), the English Channel (about 8 Bq/m3) and the

98
North Sea (about 5 Bq/m3) resulting from discharges from Sellafield and Cap de la Hague. In
1996–2000, the mean concentrations were about 10 Bq/m3 in the Baltic Sea, about 4 Bq/m3 in
the English Channel, and about 4 Bq/m3 in the North Sea.
The effective half-lives of 90Sr, 137Cs and 239,240Pu in Atlantic surface water were
calculated using data stored in the GLOMARD database, mostly based on Risö reports [111],
BSH and CEFAS (The Centre for Environment, Fisheries and Aquaculture Science, UK) data.
All data used for the calculation of effective half-lives of 90Sr, 137Cs and 239,240Pu in the
different boxes dividing the Atlantic Ocean (except for Box 19, where no data were available)
are shown in Figs 101–103 (for 90Sr), 104–106 (for 137Cs) and 107–109 (for 239,240Pu). The
calculated effective half-lives and predicted concentrations are given in Tables VI–VIII. The
values for the different boxes are very widely scattered, so it is more useful to group data for
the north, central and south Atlantic Ocean (Table XIV).
90
Sr and 137Cs show similar half-lives of 16 ± 4 and 19 ± 4 years, respectively, for the
north Atlantic, 24 ± 2 and 24 ± 6 years for the central Atlantic and 17 ± 9 and 20 ± 6 years for
the south Atlantic Ocean. The total of all Atlantic data is 22 ± 2 and 20 ± 3 years, for 90Sr and
137
Cs, respectively. The 239,240Pu data are close, giving a value for all the Atlantic Ocean of 9
± 1 year.
Data for all oceans (Table XV) gave similar effective half-lives for 90Sr and 137Cs, 19 ±
3 and 20 ± 2 years, respectively. As expected, the half-life is similar for both radionuclides,
therefore, one can accept a mean value of 19 ± 2 years. The 239,240Pu effective half-life in
surface water is 9 ± 1 year. The corresponding residence times of 90Sr (137Cs) and 239,240Pu in
surface water are 27 ± 2 and 13 ± 1 years, respectively.
In 1988–1989 the SWEDARP expedition collected surface sea water in the Atlantic
Ocean between 73°N and 72°S [112]. The samples were analysed for 137Cs and 239,240Pu and
were compared with the GEOSECS data from the expedition in 1972–1973. The effective
half-life of 137Cs was determined to be 23 years (or longer), corresponding to a mean
residence time of 33 years. The effective half-life of 239,240Pu was determined to be 7–8 years.

TABLE XIV. MEAN EFFECTIVE HALF-LIVES OF 90Sr, 137Cs AND 239,240Pu IN

ATLANTIC OCEAN SURFACE WATER
Effective half-life ± 1σ*
(year)
90 137 239,240
Area Boxes Sr Cs Pu

North Atlantic 25+28 15.6 ± 4.3 18.6 ± 4.2 9.0 ± 0.6

Central Atlantic 29 24.2 ± 2.1 23.7 ± 5.7 9.8 ± 2.9
South Atlantic 30 17.3 ± 8.8 20.2 ± 6.3 10.7 ± 4.9
All Atlantic 25–30 22.3 ± 2.4 20.4 ± 3.0 9.1 ± 0.5

* Error weighted averaged values

99
 80
18 20

60
25

40
28

20
Latitude

29
-20

-40
30

-60
13

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude

FIG. 92. Latitudinal boxes in the Atlantic Ocean.

80
190 ± 30 350 ± 290
(14) (16)

60 200 ± 40
(8)

40

20
Latitude

0
69 ± 14
(97)

-20

-40

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude

FIG. 93. 3H in Atlantic surface water (1991–1995), decay-corrected to 01.01.2000, in mBq/L.

100
 80
1.7 ± 0.6 3.5 ± 2.0
(25) (96)

11.3 ± 2.8
60 (99)
1.6 ± 1.1
(22) 5.5 ± 2.2
8.3 ± 4.3
(215)
(89)
40
1.2 ± 0.2
(19)
1.4 ± 0.1
(2)
20
Latitude

0
0.8 ± 0.1
(5)

-20

-40 0.4 ± 0.2

(2)

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude

FIG. 94. 90Sr in Atlantic surface water (1991–1995), decay-corrected to 01.01.2000, in

mBq/L.

80 3.5 ± 2.4 5.3 ± 3.5

(68) (181)

60
3.0 ± 2.0
40 ± 12
(68)
(41)

40
2.0 ± 0.3
(28)
2.4 ± 0.2
20 (2)
Latitude

1.4 ± 0.2
(2)
-20

-40 0.5 ± 0.1

(2)

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude
137
FIG. 95. Cs in Atlantic surface water (1991–1995), decay-corrected to 01.01.2000, in
mBq/L.

101
 80 6.4 ± 1.5
11 ± 12
(24)
(99)

60
13 ± 17
(32)

40

5.9 ± 2.8
(12) 16.6 ± 6
20 (2)
Latitude

2.8 ± 1.3
(5)
-20

-40
1.8

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude

FIG. 96. 239,240Pu in Atlantic surface waters (1991–1995), in μBq/L.

80

60 390
(1)

40
175 ± 12
(3)
279 ± 48
(5)
20
Latitude

-20

-40

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude

FIG. 97. 3H in Atlantic surface water (1996–2000), decay-corrected to 01.01.2000, in mBq/L.

102
 80 2.2
(1)

49 ± 83
(14)
60
2.1 ± 0.9
(17)

40
1.2 ± 0.6
(17)
1.7 ± 0.2
20 (15)
Latitude

-20

-40

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude
90
FIG. 98. Sr in Atlantic surface water (1996–2000), decay-corrected to 01.01.2000, in
mBq/L.

80 14
(1)

60 57 ± 55
4.2 ± 2.7
(28)
(16)

40
1.7 ± 0.8
(16)

2.6 ± 0.4
20 (15)
Latitude

-20

-40

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude
137
FIG. 99. Cs in Atlantic surface waters (1996–2000), decay-corrected to 01.01.2000, in
mBq/L.

103
 80

60
36 ± 16
(9)

40
5.0 ± 2.7
(17)

14 ± 4
20 (7)
Latitude

-20

-40

-60

-100 -80 -60 -40 -20 0 20 40 60 80 100

Longitude
FIG. 100. 239,240Pu in Atlantic surface waters (1996–2000), in μBq/L.

TABLE XV. MEAN EFFECTIVE HALF-LIVES OF 90Sr, 137Cs AND 239,240Pu IN SURFACE
WATER OF THE WORLD OCEAN
Effective half-life ± 1σ*
(year)
90 137 239,240
Area Boxes Sr Cs Pu

North Pacific 01-05 12.4 ± 1.1 12.7 ± 1.4 6.7 ± 0.9

Equatorial Pacific 06+07 21.1 ± 1.9 28.6 ± 3.0 10.2 ± 2.4
South Pacific 08-12 17.9 ± 1.0 22.2 ± 5.2 12.1 ± 3.6
All Pacific 01-12 15.9 ± 2.4 15.9 ± 4.3 7.4 ± 1.1

North Indian 15 20.2 ± 1.9 21.2 ± 7.6

South Indian 16+17 21.9 ± 6.3 8.8 ± 1.0
All Indian 15-17 20.3 ± 1.8 9.0 ± 1.7

North Atlantic 25+28 15.6 ± 4.3 18.6 ± 4.2 9.0 ± 0.6

Central Atlantic 29 24.2 ± 2.1 23.7 ± 5.7 9.8 ± 2.9
South Atlantic 30 17.3 ± 8.8 20.2 ± 6.3 10.7 ± 4.9
All Atlantic 25-30 22.3 ± 2.4 20.4 ± 3.0 9.1 ± 0.5

All Oceans 19.1 ± 3.2 19.8 ± 1.5 8.8 ± 1.0

* Error weighted averaged values

104
6.2. Water column radionuclide time series in the Atlantic Ocean

Sampling stations for the evaluation of 90Sr, 137Cs and 239,240Pu water profiles time series
in the Atlantic Ocean are shown in Fig 110. Corresponding 90Sr, 137Cs and 239,240Pu water
profiles in the north Atlantic Ocean (north of Iceland) are shown in Figs 111, 112 and 113,
respectively. Data for 1972 have been extracted from the GEOSECS project and for 1985 and
1995 from the BSH database. Data are fairly widely scattered for 90Sr, however, data for 1985
(except for two outliers) are lower than those for 1972. The results from 1995 are in between
the 1972 and 1985 values. Also, the 1985 values below 1000 m are much higher than for
1972. Higher 1995 values may be due to discharges from Cap de la Hague in the eighties.
137
Cs profiles clearly show increasing concentrations from 1972, to 1985 and 1995,
reflecting 137Cs releases from Sellafield. According to Dahlgaard [113] the expected transit
time from Sellafield to the investigated sites is around 10 years, which appears in good
agreement with maximum 137Cs releases in the mid-seventies. However, the further increase
in 1995 is difficult to explain.
239,240
Pu data show a remarkable decrease from a peak value of around 58 mBq/m3 in
1972 to about 13 mBq/m3 in 1995.
Another comparison of water profiles was made for 90Sr, 137Cs and 239,240Pu obtained
from the GEOSECS programme (1973) and the "Walther Herwig II" cruise of August–
September 1996 organized by Federal Research Centre for Fisheries (Germany) in which
IAEA-MEL participated. Although the positions of the stations are not the same (see Fig.
110), the 90Sr data presented in Fig. 114 show a decrease in surface water concentrations from
2 to 1 Bq/m3 and an increase below 750 m water depth in 1996 data. 137Cs data show similar
behaviour (Fig. 115).
The 137Cs/90Sr activity ratios from the 1996 data show values of around 1.5, except for
layers between 1500–1400 m, where ratios of up to 2 were observed. 239,240Pu profiles shown
in Fig. 116 clearly show the displacement of the maximum from around 600 m, observed in
1973, down to 750–1500 m in 1996. Unfortunately, there are not enough GEOSECS data to
make a more precise comparison. The remarkable 239,240Pu peak, as well as the 90Sr, 137Cs, 3H
and 14C peaks observed in deep-water layers are due to specific transport processes in the NE
Atlantic [114].

6.3. Inventories of 90Sr and 137Cs in the NE Atlantic

From 1983 to 1995 BSH collected and analysed water column samples from the NE
Atlantic. Table XVI summarizes the results of 90Sr and 137Cs inventory calculations based on
the data supplied by them. It appears that the 137Cs observations are in reasonable agreement
with the known inputs to the Atlantic Ocean, but the 90Sr observations are about double the
expected values. The explanation may be that the number of 90Sr determinations is relatively
small. But the discrepancy may also be due to the fact that the samples may not be
representative of the western and central parts of the N Atlantic.
The inventory of 137Cs in ocean sediment is in the order of 0.1–0.2 kBq/m2 i.e. about
5% of that present in the water column. Hence, sediment does not influence the inventory
estimates significantly. The reasonable agreement between observations and inputs may be
less favourable for 137Cs if one considers that the NE Atlantic contains both reprocessing and
Chernobyl 137Cs. The inventories of 90Sr and 137Cs determined from measurements of water
column samples collected in the NE Atlantic are up to twice the known inputs to the
N Atlantic Ocean. The discrepancy is higher for 90Sr than 137Cs.

105
6.4. Radionuclides in northern European seas

The northern European seas have received input of anthropogenic radionuclides from
different sources, mainly :

(i) Global fallout,

(ii) Liquid discharges from European nuclear reprocessing plants at Sellafield and
Cap de la Hague,
(iii) Fallout from the accident at Chernobyl.

In addition to these sources, nuclear power stations, fuel production facilities, nuclear
research facilities, and dumping of low level radioactive waste in the deep NE Atlantic Ocean
may contribute to the contamination of the immediate environment. The discharges or
releases from these sources are not detectable in the open marine environment and their
impact on the local environment is monitored regularly by the competent authorities.
90 137
TABLE XVI. WATER COLUMN INVENTORIES OF Sr AND Cs IN THE NE
ATLANTIC IN THE YEAR 2000

Year BoxNo. Columns Year 1 SD N Atlantic Area Inventory Atlantic INV/INP

2000 latitude (1012m2) (PBq) input
mean (PBq)
(kBq/m2)
137
Cs
1985 25 5 3.16 0.64
1995 25 4 3.26 0.51
Mean 25 3.21 0.07 70º-60º N 4.560 14.6 16.8 0.87
1985 18 9 4.67 1.66
1995 18 6 4.84 0.67
Mean 4.76 0.12 80º-70º N 3.369 16.0 13.1 1.22
1983 28 7 3.05 0.21
1984 28 10 3.34 0.27
1985 28 3 3.29 0.33
Mean 3.23 0.16 60º-30º N 20.842 67.3 48.3 1.39
90º-30º N 28.771 97.9 78.2 1.25
90
Sr
1985 25 2 2.01 0.43 70º-60º N 4.560 9.2 4.5 2.04
1985 18 3 2.58 1.53 80º-60º N 3.369 8.7 2.2 3.95
1983 28 1 2.62
1984 28 5 2.07 0.24
Mean 2.35 0.39 60º-30º N 20.842 48.9 24.2 2.02
90º-30º N 28.771 66.7 30.9 2.16

NOTE: The inputs from reprocessing and Chernobyl were assumed by the year 2000 to have
been equally divided between the three Atlantic boxes. Any input to the Arctic Ocean was
neglected.

In the Arctic Ocean various additional potential sources exist, such as: dumped
radioactive waste in the Kara and Barents Seas [12, 115]; discharges from nuclear activities
on the Kola peninsula; the sunken nuclear submarine "Komsomolets"; plutonium
contamination at the Thule, Greenland, accident site.

106
 Box 18 Box 20
100 100

10 10

Sr (mBq/L)
Sr (mBq/L)

90
1

90
1

0.1
0.1
1950 1960 1970 1980 1990 2000
1950 1960 1970 1980 1990 2000
Year Year

Box 21 Box 22
100 100

10 10

Sr (mBq/L)

Sr (mBq/L)
90
1

90
1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 101. 90Sr surface water time series in the Atlantic Ocean.

107
 Box 23 Box 24

108
1000 100

100 10

Sr (mBq/L)

Sr (mBq/L)
90

90
10 1

1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 25
Box 26
100 100

10 10

Sr (mBq/L)
Sr (mBq/L)

90
90
1 1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

90
FIG. 102. Sr surface water time series in the Atlantic Ocean.
 Box 27 Box 28
100 100

10 10

Sr (mBq/L)
Sr (mBq/L)

90
90
1 1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 29 Box 30
100 100

10 10

Sr (mBq/L)

Sr (mBq/L)
90
1

90
1

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

90
Fig. 103. Sr surface water time series in the Atlantic Ocean.

109
 Box 18 Box 20
100 100

110
10 10

Cs (mBq/L)
Cs (mBq/L)
1

137
1

137
0.1
0.1
1950 1960 1970 1980 1990 2000
1950 1960 1970 1980 1990 2000
Year Year

Box 21 Box 22
1000 1000

100
100

10

Cs (mBq/L)
Cs (mBq/L)
10

137
137
1

0.1 1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 104. 137Cs surface water time series in the Atlantic Ocean.
 Box 23 Box 24
1.E+05 100

1.E+04

1.E+03
10
1.E+02

1.E+01

Cs (mBq/L)
Cs (mBq/L)

137
1

137
1.E+00

1.E-01

1.E-02 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 24 Box 26
100 1000

10 100

Cs (mBq/L)

Cs (mBq/L)
1 137
10

137
0.1 1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

137
FIG. 105. Cs surface water time series in the Atlantic Ocean.

111
 Box 27 Box 28
100 100

112
10 10

Cs (mBq/L)
Cs (mBq/L)
1

137
1

137
0.1
0.1
1950 1960 1970 1980 1990 2000
1950 1960 1970 1980 1990 2000
Year Year

Box 29 Box 30
100 100

10 10

Cs (mBq/L)
Cs (mBq/L)
1 1

137
137

0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

137
FIG. 106. Cs surface water time series in the Atlantic Ocean.
 Box 18 Box 20
100 100

10 10

Pu (µBq/L)

Pu (µBq/L)
1 1

239+240

239+240
0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 21 Box 22
100 100

10 10

Pu (µBq/L)

Pu (µBq/L)
1 239+240 1

239+240
0.1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 107. 239,240Pu surface water time series in the Atlantic Ocean.

113
114
Box 23 Box 24
100 1000

10 100

Pu (µBq/L)
No Data

Pu (µBq/L)
1 10

239+240
239+240
0.1 1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 25 Box 26
1000 100

100 10

Pu (µBq/L)
No Data

Pu (µBq/L)
10 1

239+240
239+240

1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 108. 239,240Pu surface water time series in the Atlantic Ocean.
 Box 27 Box 28
1000 100

100 10

Pu (µBq/L)
Pu (µBq/L)
10 1

239+240
239+240
1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

Box 29 Box 30
1000 100

100 10

Pu (µBq/L)
Pu (µBq/L)
10 1

239+240
239+240

1 0.1
1950 1960 1970 1980 1990 2000 1950 1960 1970 1980 1990 2000
Year Year

FIG. 109. 239,240Pu surface water time series in the Atlantic Ocean.

115
116
80

BSH
BSH
G
BSH
60 G

B-1 B-0T-115
B-3 M-525

40 M-521

Latitude
T-112

G G

20

0
-60 -40 -20 0 20
Longitude

FIG. 110. Vertical profile stations in the North Atlantic (G-GEOSECS sites, BSH-BSH sites, B-IAEA sites).
 90
Sr(mBq/L)
0 1 2 3 4
0

500

1000

1500
Depth(m)

2000

2500

3000 1972
1985
1995

3500

FIG. 111. 90Sr water profiles time series in the North Atlantic (north of 60°N).

137
Cs(mBq/L)
0 1 2 3 4 5
0

500

1000

1500
Depth(m)

2000

2500

3000 1972
1985
1995

3500

FIG. 112. 137Cs water profile time series in the North Atlantic (north of 60°N).

117
 239+240 3
Pu(mBq/m )
0 10 20 30 40 50 60
0

500

1000

1500
Depth(m)

2000

2500

3000 1972
1995

3500

FIG. 113. 239,240Pu water profile time series in the North Atlantic (north of 60°N).

90
Sr(mBq/L)
0 0.5 1 1.5 2 2.5
0

500

1000
Depth(m)

1500

2000

2500
GEOSECS(1973)
IAEA B1(1996)

3000

FIG. 114. 90Sr water profile time series in the North Atlantic (south of 50°N).

118
 137
Cs(mBq/L)
0 1 2 3 4
0

500

1000

Depth(m)

1500

2000
GEOSECS-???(1973)
IAEA B1(1996)

2500

FIG. 115. 137Cs water profile time series in the North Atlantic (south of 50°N).

239+240 3
Pu(mBq/m )
0 10 20 30 40 50 60
0

500

1000
Depth(m)

1500

2000

GEOSECS(1973)
IAEA B1(1996)
2500

FIG. 116. 239,240Pu water profile time series in the North Atlantic (south of 50°N).

119
 2.0
1.5
2.2

4.5 4.3

6.3

2.6

8.8

2.4
5.8

18
2.8 4.0 2.8 2.5
43
18 66
21 45 3.8 2.9 2.6
27 334
42
21 3.3 3.3 3.0 3.1 2.6 3.2
17 9.6
2.3 2.8
13 2.3

3.5 2.0 2.2

3.5
3.6 1.9 2.4 2.2

2.2
90
2.2 Sr [Bq/m³]
2.0
November 1999
1.7
1.7
Surface, 0 - 10 m Layer
1.7
Subsurface , close to seabed
Bundesamt für Seeschiffahrt und Hydrographie, Hamburg & Rostock

FIG. 117. 90Sr distribution in water of the Irish and North Seas, including the English
Channel in November, 1999. The relative uncertainty for the data is less than 5%.

3.0
2.2
3.6

9.1 6.6
6.6
8.6
3.9
12.0
5.9
4.4 4.7

16.8

17.9 4.9
6.0
15.7
5.3 4.4
11.8

38.4
5.5 7.4 8.1 6.4 3.6
111
41.7 151
37.3 48.1 123 8.2 6.7 3.9
202 112
25.1 29.3 68.2 145
20.2 19.0 22.9 52.6 112 6.5 6.6 5.2 3.9 4.0 3.4
22.7 13.5 21.2 135 3.4 3.7
12.0 28.6 27.1 3.4

7.2 3.0 3.1

7.2
3.6 3.8
7.6 3.4

2.2 3.2
137
3.3 Cs [Bq/m³]
2.4
2.4
November 1999
2.7 2.8 2.9
Surface, 0 - 10 m Layer
2.1 2.5
2.6
Subsurface , close to seabed
Bundesamt für Seeschiffahrt und Hydrographie, Hamburg & Rostock

FIG. 118. 137Cs distribution in water of the Irish and North Seas, including the English
Channel, in November 1999. The relative uncertainty for the data is less than 5%.

120
FIG. 119. 137Cs in surface water of European seas (1976–1980).

FIG. 120. 137Cs in surface water of European seas (1981–1985).

121
 FIG. 121 137Cs in surface water of European seas (1986–1990).

FIG. 122. 137Cs in surface water of European seas (1991–1995).

122
10000

Elbe1
Bq/m³
Borkumriff

1000

100

10

1
61 65 69 73 77 81 85 89 93 97

FIG. 123. Temporal trend of 137Cs concentrations at two locations in the inner German Bight.
This area is influenced by La Hague discharges.

30

20

y = -0.0043x + 162.67
Bq/m³

R2 = 0.8629

y = 659056.7946996e-0.0003098x
10
R2 = 0.8420107

0
May-90 Sep-91 Jan-93 Jun-94 Oct-95 Mar-97 Jul-98 Dec-99 Apr-01
time

FIG. 124. Temporal trend of 137Cs concentrations in the outer German Bight (55°N, 6°E).
This location is influenced by Sellafield discharges.

123
 Several cruises have recently been organized to northern European seas mainly by
Germany and the UK [116–119].

6.4.1. The Irish Sea

The Irish Sea (Box 23) was recently monitored for 90Sr, 137Cs and 99Tc in the autumn of
1999 by BSH on a cruise by the R/V "Gauss" in co-operation with British and Irish scientists.
The distribution of the activity concentrations are given in Figs 117 and 118 for 90Sr and
137
Cs, respectively.

The different sources of 90Sr and 137Cs in the Irish Sea can be identified by the activity
ratio 137Cs/90Sr. It becomes evident that the only position, where the typical discharge ratio as
given by BNFL [120] is found is directly at the discharge area, where 137Cs/90Sr = 0.6. In
other areas this ratio is significantly different, proving that resuspension of sediment is the
dominant source of 137Cs at present in the Irish Sea.

As the distribution of 90Sr, 137Cs and 239,240Pu (Tables VI–VIII) in the Irish Sea has been
controlled by discharges, effective half-lives were not calculated. The average 90Sr, 137Cs and
239,240
Pu concentrations in the Irish Sea in the year 2000 have been estimated to be 50 Bq/m3,
60 Bq/m3 and 500 mBq/m3, respectively.
137
Cs concentrations in surface water grouped for the periods 1976–80, 1981–85, 1986–
90 and 1991–95 are shown in Figs 119, 120, 121 and 122, respectively, clearly indicating
transport of 137Cs from Sellafield reprocessing plant.

6.4.2. The North Sea

The North Sea (Box 22) receives contamination from the reprocessing plants at
Sellafield and Cap de la Hague by the prevailing residual currents from the Irish Sea and the
English Channel. Consequently, the concentrations of 137Cs, 90Sr and other radionuclides
follow with delay the temporal trends of the discharges. The maximum discharge of 137Cs and
other ß-emitting nuclides at Sellafield occurred in 1975; the highest concentrations of 137Cs
were measured around 1979 in the North Sea, with values of about 500 Bq/m3. After 1975,
the discharges decreased steadily as mentioned in Chapter 2.2. Due to significantly decreasing
discharges in recent years, the concentrations of 137Cs, 90Sr and transuranics are presently only
slightly above the global fallout levels for North Atlantic surface water. Remobilization of
137
Cs from highly contaminated sediment in the Irish Sea is now the dominant source also for
water contamination of the North Sea [121]. Levels of 137Cs in November 1997 were between
3.5 Bq/m3 in the southeastern North Sea and 12.4 Bq/m3 in the central southern North Sea.
The concentrations of 90Sr were between 2.3 and 4.2 Bq/m3 in the south, with lower levels in
the north.

The general downward trend over recent years of 90Sr and 137Cs can be seen at several
locations in the North Sea. This is due to both the physical decay of the global fallout level,
decreasing discharges from the reprocessing plants at Sellafield and Cap de la Hague, as well
as transport of these radionuclides to the north. The trend at two positions in the German
Bight is shown in Fig. 123, whereas the outer German Bight (55°N, 6°E) reflects more the
contamination from Sellafield about three years after the release into the Irish Sea (Fig. 124).

The Sellafield signal can also be detected in the North Sea for transuranic elements; the
highest levels were found near the Scottish coast with 239,240Pu concentrations of up to 55
mBq/m³ in Pentland Firth in 1997. The concentrations decrease along the British east coast to

124
the southern central North Sea, where levels of less than 20 mBq/m³ are found. In the German
Bight the values are even less than 10 mBq/m³. The activity ratio of 238Pu/239,240Pu in the
southern North Sea indicates a source of plutonium other than the Cap de la Hague plant,
where the ratios are sometimes even higher than unity. In general, the activity ratios in the
whole area indicate that the reprocessing plants are the dominant source of plutonium.

The 3H, 90Sr, 137Cs and 239,240

Pu surface water time series are shown in Figs 101, 104
and 107, respectively.

Combining all available data for 90Sr, 137Cs and 239,240Pu, the effective half-lives could
be calculated (keeping in mind that they could have been affected by releases from
reprocessing plants and the Chernobyl accident (Tables VI–VII)). The effective half-lives for
90
Sr and 137Cs are 6.9 ± 0.4 and 5.7 ± 0.3 years, respectively. The 239,240Pu value is not
sufficiently precise (24 ± 17 years). The average 90Sr, 137Cs and 239,240Pu concentrations,
estimated from recent measurements, are for 2000: 4, 4.5 Bq/m3 and 15 mBq/m3, respectively.

6.4.3. The Baltic Sea

The accident at Chernobyl deposited large quantities of radionuclides over the northern
part of the Baltic Sea (Box 21). The levels of 137Cs in the Baltic Sea (Fig. 125; [122]) were
dominated by this fallout from 1986 onwards [5]. Before 1986, 137Cs was due to global fallout
and the inflow of North Sea water through the Danish Straits. Since 1986, a great proportion
of 137Cs was deposited in the fine grained sediment of the Baltic Sea. The inventory in the
water phase has decreased by about a factor of 2 since then. The concentrations of 90Sr have
remained fairly unchanged over the years and are in the range between 10 and 15 Bq/m³ in
surface water of the Baltic Sea. The main source of this radionuclide is global fallout, whereas
the activity ratio of 137Cs/90Sr is not typical due to certain inputs from rivers. This mechanism
is almost negligible for 137Cs.

Due to the permanent halocline in the Baltic Sea there still exists a significant difference
in the concentrations of 137Cs in surface water and in the deeper layers below the halocline.
This is true in particular for the Belt Sea (western Baltic) where the inflow from the North Sea
with lower levels occurs below the halocline and the outflow of low salinity water at the
surface carries higher contamination levels. In addition, Chernobyl fallout was very unevenly
distributed. However, mixing of water masses has led to a more homogeneous distribution in
different parts of the Baltic over years. The temporal trend in 90Sr and 137Cs concentrations at
one station in the western Baltic Sea is shown in Fig. 126.

The 90Sr, 137Cs and 239,240Pu surface water time series are given in Figs 101, 104 and
107, respectively. The calculated effective half-lives for 90Sr, 137Cs and 239,240Pu in the Baltic
Sea are 12.0 ± 1.7, 14.1 ± 1.8 and 4.9 ± 1.4 years, respectively. The average concentrations of
90
Sr, 137Cs and 239,240Pu in surface water estimated from recent measurements for the year
2000 are around 10 Bq/m3, 60 Bq/m3 and about 3 mBq/m3, respectively (Tables VI–VIII).

6.4.4. The Arctic Seas

The Arctic Seas (the Norwegian, Barents and Kara Seas) were recently investigated in
detail in order to study potential transport of radioactive contaminants from nuclear dumpsites
in the Kara and Barents Seas into the NE Atlantic [12, 115]. The levels of 137Cs were
significantly

125
126
FIG. 125. 137Cs contours of Baltic Sea surface waters after the Chernobyl accident (for the period 1986–1988) as extracted from the GLOMARD
database.
 1000

Cs-137
Bq/m³
Sr 90

100

10

1
61 65 69 73 77 81 85 89 93 97

FIG. 126. Temporal trends of 137Cs and 90Sr in the western Baltic Sea.

Bq/m3
50

40

30

20

10

Cs-137

Sr-90

90 137
FIG. 127. Sr and Cs in Barents Sea surface water as extracted from the GLOMARD
database.

127
FIG. 128. 137Cs contours of western Black Sea surface water after the Chernobyl accident in
1988, as extracted from the GLOMARD database.

significantly lower than in 1985 due to lower levels in the North Sea as a consequence of
decreased discharges at Sellafield. It was also found that at deeper water layers, Sellafield-
derived transuranics identified by their activity ratios are transferred into the Norwegian Sea
[123].

In Arctic waters there is no indication of long range contamination from nuclear wastes
and other radioactive objects dumped by the former USSR. Samples taken in its vicinity
during 1992 and 1995 indicate that there is also no long range contamination from the sunken
nuclear submarine "Komsomolets" in the northern Norwegian Sea. Except for global fallout,
the main source of radionuclides in the Arctic Seas remains the contributions from nuclear
reprocessing plants. Fig. 127 confirms this statement showing the time evolution of 90Sr and
137
Cs activities in Barents Sea surface water.

The distribution maps and average 90Sr, 137Cs and 239,240Pu concentrations for the Arctic
Seas are given in Figs 94–96 for 1991–1995 and 98–100 for 1996–2000, respectively. The
corresponding time series (Box 20) are shown in Figs 101, 104 and 107. The calculated
effective half-lives for 90Sr, 137Cs in the Barents Sea are 5.8 ± 0.5 and 4.2 ± 0.2 years,
respectively. The average 90Sr, 137Cs and 239,240Pu concentrations estimated from recent
measurements are for the year 2000 around 2 and 3 Bq/m3, and 20 mBq/m3, respectively
(Tables VI–VIII).

6.5. Radionuclides in the Mediterranean Sea

The Mediterranean Sea is an enclosed, deep basin that communicates with the Atlantic
Ocean through the narrow, shallow Strait of Gibraltar. Here a surface flux of Atlantic, low
salinity water (36–36.5‰) enters the Mediterranean Sea, while a subsurface water mass,
characterized by salinity higher than 37.5‰ leaves the basin. The entire Mediterranean is a
concentration basin, with evaporation exceeding precipitation and runoff. Due to the increase
in salinity and consequent density instabilities, deep and intermediate waters are formed by
vertical convection at some key sites, as discussed below.

128
 The general circulation of the basin is complex and can be summarized as follows: the
major phenomenon influencing the surface circulation is the Atlantic water entering via the
Strait of Gibraltar. After some meandering in the Alboran Sea, this water mass proceeds
eastward, along the north African coast. After crossing the Sicilian Sill, the Atlantic stream
occupies the southern part of the Ionian Sea, becoming an intensified mid-Mediterranean jet.
In the area between Crete and Rhodes, extensive vertical convection gives rise to the
formation of the saltier and denser Levantine Intermediate Water (LIW) that stabilizes at 200–
600 m depth, moves westward and passes over the Sicilian Sill into the western basin. After
following a rather complicated path throughout the basin, the LIW finally flows, mixed with
some Western Mediterranean Deep Water, out of the Mediterranean, crossing the Strait of
Gibraltar at an average depth of more than 150 m.

The deepest Mediterranean water is mainly formed in areas where prolonged periods of
cold winds sharply increase the evaporation rates and produce, at the surface, a dense, cold,
well oxygenated water mass that sinks rapidly, reaches the bottom and spreads all over the
basin.

The Gulf of Lions, the Liguro-Provençal Basin, the Adriatic and the Cretan Seas have
been identified as the most important sites for deep-water formation. More recently, important
changes have been registered in deep-water formation and circulation in the Eastern Basin,
with deep and intermediate water masses also being formed in the Aegean Sea.

The major source of anthropogenic radionuclides to the Mediterranean Sea is fallout

from atmospheric weapons testing in the early sixties (12 PBq of 137Cs and 0.19 PBq of
239,240
Pu) [124–126]. Fallout from the Chernobyl accident contributed significantly to the total
input of caesium isotopes. It is estimated that 3 to 5 PBq of 137Cs were deposited after the
accident, mainly in the eastern and northern parts of the basin. An additional input of
Chernobyl radionuclides came through the Black Sea (0.3 PBq of 137Cs) [127]. Figure 128
documents the 137Cs levels in the western Black Sea in 1988 as obtained from the
GLOMARD database [128]. The input deriving from the nuclear industry is very small
compared to other sources. The Marcoule (France) reprocessing plant is authorized to
discharge low level effluents into the Rhone river which flows into the NW Mediterranean.
The discharges up to 1995 amount to a total of 30.2 TBq of 137Cs and 0.26 TBq of plutonium
isotopes.

6.5.1. Surface water radionuclide time series

No time series stations have been established in the Mediterranean Sea for
anthropogenic radionuclide concentrations in open waters. However, Fukai et al. [129]
showed that before the Chernobyl accident there were no significant differences in surface
137
Cs concentrations in the different basins of the Mediterranean Sea. In 1977, the mean
values ranged from 4.4 ± 0.7 Bq/m3 in the SW Mediterranean and in the Tyrrhenian Sea, to
4.8 ± 1.8 Bq/m3 in the NW Mediterranean, Adriatic and Ionian Seas. Slightly lower values
were found only in the SE Mediterranean basin (4.2 ± 0.3 Bq/m3).

Also for plutonium, the few studies conducted over the whole of the Mediterranean, did
not show significant differences in the levels measured in open surface water of the different
basins [130], while there were some noticeable differences between the open sea and coastal
areas [131].

129
 It is thus reasonable to calculate the time trend of anthropogenic radionuclide
concentrations in surface sea water using average annual values obtained in different areas of
the Mediterranean Sea.

The time trend of 137Cs concentrations in surface sea water is shown in Fig. 129. An
exponential decrease is apparent in the period 1970–1985. In 1986, Chernobyl fallout deeply
modified 137Cs distribution in the Mediterranean, producing a significant increase in the levels
of the northern and eastern basins. 137Cs concentrations were back to pre-Chernobyl values
over the entire Mediterranean Sea in 1990.

Figure 130 shows the plutonium time trend over the period 1970–1997. As for caesium,
there is a clear exponential decrease in concentrations. The calculated effective half-life for
239,240
Pu is 13 ± 2 years and the corresponding mean residence time is about 19 years. These
data are in reasonable agreement with the residence times of 12 years [132] and 20–30 years
[106] calculated by other methods. As expected, these parameters are slightly lower than
those derived for caesium, as plutonium is removed from the surface layer not only by
physical processes, but also by association with sinking organic and inorganic particles.

Four main data sets were analysed to estimate recent radionuclide concentrations: the
first obtained by Papucci and Delfanti for the eastern Mediterranean in 1995–97 [133], the
second by BSH for the western Mediterranean in 1997 [136], the third for the Strait of
Gibraltar in 1997, and the fourth in the framework of the WOMARS project (ITALICA
cruise) for the eastern Mediterranean in 1998 [135].
137
Cs concentrations range from 2.5 Bq/m3 in the low salinity Atlantic water inflow to
an average value of 3.1 Bq/m3 in the eastern Mediterranean. For 90Sr there are no significant
differences between the two basins (1.8 ± 0.2 Bq/m3). For plutonium, data are available only
for the western Mediterranean. The mean concentrations of anthropogenic radionuclides in
Mediterranean surface water are given in Table XVII.
239,240
Pu concentration (around 12 mBq/m3) for the reference date of January 1st, 2000
was estimated using the effective half-life of 11 years obtained from the analysis of the time
trend evolution of its concentration in the period 1970–1994. The average 137Cs concentration
(around 2.6 Bq/m3) was estimated using the recent data, because 137Cs effective half-life could
not be determined for the period following the Chernobyl accident. The same approach was
adopted for 90Sr (the average concentration is around 1.7 Bq/m3).

TABLE XVII. MEAN CONCENTRATION OF ANTHROPOGENIC RADIONUCLIDES IN

SURFACE WATER OF THE MEDITERRANEAN SEA

Radionuclide Year Area Mean St. No. of Decay

concentration dev. data corrected
for 2000
(Bq/m3) (Bq/m3)
137
Cs 1995 E. Med. 3.4 0.5 5 3
137
Cs 1997 W. Med., Gibraltar 2.5 0.2 13 2.4
137
Cs 1998 E. Med. 3.1 0.1 4 3
90
Sr 1997–98 All Med. 1.8 0.2 6 1.7
239,240
Pu 1997 W. Med. 0.012 0.003 10 0.012
238
Pu 1997 W. Med. 0.002 0.001 10 0.002
241
Am 1997 W. Med. 0.0014 0.0001 3 0.001

130
6.5.2. Recent data on 137Cs and 239,240Pu in the water column of the Mediterranean Sea

Only a few data are available for the period 1995–2000 on radionuclide vertical profiles
in the Mediterranean Sea. The two main data sets published to date concern the eastern
Mediterranean and the Strait of Gibraltar.

Eastern Mediterranean

The eastern Mediterranean has been studied in detail, also in relation to the so-called
"deep water transient", the change in circulation of the deep and intermediate water that made
the basin of interest in the 1990s [150]. A first analysis of radionuclide data was published by
Papucci and Delfanti [133], who discussed the present distribution in relation to water
circulation and to the input of Chernobyl radionuclides. The data were collected in 1995 and
1996–97. The surface concentration of 137Cs ranged between 3.3 and 4.0 Bq/m3. The vertical
profiles showed relative maxima in recent intermediate and deep water, also characterized by
an increase in dissolved oxygen concentration. Figure 131 shows 137Cs vertical profiles at 4
stations in the Ionian Sea and southeastern Mediterranean in 1995–96.

Strait of Gibraltar

The Strait of Gibraltar is a narrow and shallow strait that separates the Mediterranean
Sea from the Atlantic Ocean. Vertical profiles of 137Cs and 239,240Pu were determined here in
order to estimate radionuclide fluxes between the Atlantic Ocean and the Mediterranean Sea
[134]. In this area, low salinity (S=36.0-36.5‰) water enters the Mediterranean Sea in the
surface layer, at a flux of 0.72 Sv, while an almost equal amount (0.68 Sv) of saltier
(S>37.5‰) and denser water leaves the basin [151]. Radionuclide concentrations were
determined in the two different water masses near the Gibraltar Sill. The results are shown in
Table XVIII.

TABLE XVIII. CONCENTRATIONS OF ANTHROPOGENIC RADIONUCLIDES AT

THE STRAIT OF GIBRALTAR (MEAN VALUES, JUNE AND SEPT. '97)

Radionuclide AW inflow MW outflow

(S 36.0-36.5‰) (S > 37.5‰)
239,240
Pu 10.0 ± 2.5 mBq/m3 21.8 ± 2.3 mBq/m3
137
Cs 2.6 ± 0.3 Bq/m3 2.4 ± 0.3 Bq/m3

There are no significant differences in 137Cs concentrations in the waters leaving and
entering the Mediterranean Sea. As a consequence, the input flux of 137Cs to the
Mediterranean Sea is balanced by the output to the Atlantic Ocean. The present situation is
markedly different from that reported for the past, when surface concentrations were much
higher than in deep water. The net annual input of 137Cs to the Mediterranean appears to be
markedly reduced compared to 1988 (120 TBq/y) [125]. In contrast, the levels of 239,240Pu are
considerably different in the water entering and leaving the Mediterranean Sea: about
10 mBq/m3 in the Atlantic inflow and 22 mBq/m3 in the Mediterranean outflow. The net
annual output of 239,240Pu from the Mediterranean to the Atlantic is presently 0.34 TBq/y,
about one third of the value estimated in 1988. This is due to the vertical transport of
plutonium and the consequent decrease of its concentration at intermediate depths.

131
 10 137 -0.073(x-1969)
Cs = 7.9 e
9

Cs-137 (Bq/m ) 7
3

0
1965 1970 1975 1980 1985 1990 1995 2000
Year

FIG. 129. Time trend of 137Cs concentrations in surface water of the Mediterranean Sea,
1969–1998. Data from [129, 131, 133, 136–140].

70 239,240 -0.06(x-1970)
Pu = 53 e
60

50
Pu (mBq m )
-3

40

30
239,240

20

10

-10
1970 1975 1980 1985 1990 1995
Year

FIG. 130. Time trend of 239,240Pu in surface seawater of the Mediterranean Sea, 1970–1997.
Data from: [106, 131, 141–149].

132
 The most recent vertical profiles of 239,240Pu in the deep Mediterranean Sea [149] were
measured in the Alboran Sea and the Algerian Basin in 1994. They show increasing
concentrations from surface to a depth of 300–600 m and almost constant values from this
depth to the bottom. In the vertical profiles measured in the 1970s and 1980s, maximum
plutonium concentrations, found between 100–400 m depth, were higher by a factor of two
than the present levels.

6.5.3. Water column radionuclide time series

The time trend of the vertical profiles of 137Cs in the water column of the Mediterranean
Sea has been analysed, based on published data [129, 131, 136, 140].

The average vertical profiles of 137Cs for the period 1970–1982 (decay-corrected to
1994) and 1992–94 are compared in Fig. 132. While the 137Cs concentration has not
significantly changed in the depth interval 0–400 m, there has been a clear increase in the
deeper layers. The inventory corresponding to a water depth of 2700 m was about 3 kBq/m2 in
the period 1970–82 and increased to about 6 kBq/m2 in 1994, reflecting vertical transport to
the deep sea by diffusion and convection processes and, to a lesser extent, additional input
from the Chernobyl accident.

The time trend of plutonium vertical profiles has recently been analysed in detail [106].
They have shown that deep-water column (0–2000 m) inventories have not substantially
changed over the period 1976–1990, but the inventory at a given depth in the deeper layers
has increased considerably, demonstrating the slow downward movement of plutonium. The
increase at depth is almost completely balanced by the decrease in the upper mixed layer (0–
200 m). As an example, Fig. 133 shows the vertical profiles of 239,240Pu in the NW
Mediterranean in 1976 and 1990 [106, 130].

6.5.4. Radionuclide inventories in the water column of the Mediterranean Sea

137
Cs inventories in the water column have been calculated from the vertical profiles
determined in the period 1995–97 in the eastern Mediterranean by Papucci and Delfanti [133].
The inventories have been calculated by simply integrating the concentration profiles,
assuming a linear variation in concentration between sampling depths. The inventories range
between 4.2 and 9.8 kBq/m2, for water depths from 2000 to 4000 m.

These new data were combined with those obtained in the western Mediterranean in the
period 1991–94 [140, 152] and plotted versus depth. All inventories were decay-corrected to
the reference date of 2000. A linear increase in inventories with depth is evident (Fig. 134).

Plutonium and americium inventories in the Mediterranean Sea have been discussed in
detail in two recent papers [106, 149].

Leon Vintrò et al. [149] discussed the relationship between water depth and plutonium
inventories, using data obtained in the period 1990–94 (Fig. 135). The figure has been
updated, adding a small number of data obtained in the Mediterranean in 1997 [134]. Based
on the conclusions of Fowler et al. [106], who show that plutonium inventories in the water
column of the Mediterranean Sea have not significantly changed in the depth interval 0–
2000 m over the period 1976–1990, one can assume that these inventories are representative
also for the period covered by the WOMARS programme (1995–2000).

133
 Theta (°C)

A B

—Theta (°C) — Theta (°C)

C D

137
FIG. 131. Salinity, temperature, dissolved O2 and Cs vertical profiles in the eastern
Mediterranean, 1995.

134
 -3
Cs-137 (Bq m )
0 1 2 3 4 5 6
0

500

1000
Depth (m)

1500 1992-94
1970-82

2000

2500

3000

FIG. 132. Mean vertical profiles of 137Cs in the water column of the Mediterranean Sea in
1970–82 (decay-corrected to 1994) and in 1992–94.

-3
Pu-239,240 (mBq m )
0 10 20 30 40 50
0

-500

-1000
Depth (m)

Aug 1976
Nov 1989
-1500

-2000

-2500

239,240
Fig. 133. Vertical profiles of Pu in the Northwestern Mediterranean in 1976 and 1989
(data from [106, 130]).

135
 10

Cs (Bq m ) 8
-2

4
137

0
0 1000 2000 3000 4000
Water depth (m)

137
FIG. 134. Relationship between Cs inventory and water depth (data from [133, 139, 140,
152] decay-corrected to 2000).

FIG. 135. Relationship between plutonium inventories and water depth in the Mediterranean
Sea (1990–1994), data from [134, 147–149].

136
6.5.5. Radionuclide inventories in the deep Mediterranean Sea
Radionuclide concentrations and inventories are highly variable in the Mediterranean
Sea, highest on the continental shelf and near river mouths and lowest in deep-sea
environments.
Only a few studies have been conducted on radionuclides in deep-sea sediment.
Livingston et al. [153] determined the inventories of 137Cs and 239,240Pu in sediment cores
collected in the Western Mediterranean and Ionian Sea in 1975. 137Cs inventories ranged from
90 to 260 Bq/m2 and 239,240Pu inventories from 2 to 7 Bq/m2.
Studies conducted in the 1990s in the western Mediterranean [140, 154] indicate
inventories very similar to those reported in 1975: 230 Bq/m2 for 137Cs and 3 Bq/m2 for
239,240
Pu.

7. CONCLUSIONS

The aim of the WOMARS CRP was to:

(i) Identify the major sources of anthropogenic radionuclides in the world's oceans,
(ii) Develop the knowledge of the distribution of key radionuclides (90Sr, 137Cs and
239,240
Pu) in the water column and in sediment,
(iii) Study the development with time of radionuclide concentrations in water.

Three anthropogenic radionuclides, 90Sr, 137Cs and 239,240Pu were chosen as the most
important and radiologically typical of each class of marine radioactivity. They are the most
abundant anthropogenic radionuclides present in the marine environment and could lead to
the highest radiation doses to humans and marine biota.

The results confirm that the dominant source of anthropogenic radionuclides in the
marine environment is global fallout. The total 137Cs input from global fallout was estimated
to be 311 PBq for the Pacific Ocean, 201 PBq for the Atlantic Ocean, 84 PBq for the Indian
Ocean and 7.4 PBq for the Arctic Ocean. For comparison, about 40 PBq of 137Cs was released
to the marine environment from Sellafield and Cap de la Hague reprocessing plants. The
Chernobyl accident contributed about 16 PBq of 137Cs into seas, mainly the Baltic and Black
Seas where the present average concentrations of 137Cs in surface water were estimated to be
about 60 and 25 Bq/m3, respectively, while the worldwide average concentration due to global
fallout was about 2 Bq/m3.
Figure 136 and Tables XIX–XXI show the best estimates of averaged 90Sr, 137Cs and
239,240
Pu concentrations in the world's oceans and seas adjusted to the year 2000. As expected,
the highest concentrations were observed in European Seas and the lowest in the Southern
hemisphere, especially in the Antarctic Ocean.
For the purposes of this study, the world ocean was divided into latitudinal belts, for
which average radionuclide concentrations were estimated. Further, where available, time
trends in radionuclide concentrations in surface water were studied and mean residence times
of radionuclides in these areas as well as in the world ocean were estimated. The results
confirm similar residence times for 90Sr and 137Cs in surface water, varying from 11 to 30
years and from 5 to 15 years for 239,240Pu.
The mean residence times of radionuclides in surface water are listed in Table XXII.

137
138
239+240 137 90
Pu (μBq/L) Cs (mBq/L) Sr (mBq/L)

0.1
1
10
100
0.1
1
10
100

0.1
1
10
100
1000
Baltic Sea Irish Sea
Irish Sea Irish Sea Black Sea
North N. Atlantic Black Sea Baltic Sea
Barents Sea Arctic Ocean English Channel
North Sea North Sea North Sea
Med. Sea North N. Atlantic Arctic Ocean
English Channel English Channel North N. Atlantic
Japan Sea Barents Sea Barents Sea
Arctic Ocean Japan Sea Med. Sea
Black Sea
Med. Sea Japan Sea
N. Atlantic

Seas
Seas

N. Pacific N. Pacific
Baltic Sea

Seas
Indian Ocean Eq. Pacific
N. Pacific
Eq. Pacific N. Atlantic
Eq. Pacific
N. Atlantic Indian Ocean
Indian Ocean
Arabian Sea Arabian Sea
C. Atlantic
C. Atlantic S. Pacific
S. Pacific
Arabian Sea S. Pacific C. Atlantic

S. Atlantic Sth. Ocean Sth. Ocean

S. Ocean S.Atlantic S. Atlan
Antarctic Antarctic Antarctic

FIG. 136. 90Sr, 137Cs and 239,240Pu in the world's oceans and seas (adjusted to 01.01.2000).
TABLE XIX. 90Sr IN SURFACE WATER OF THE WORLD'S OCEANS AND SEAS
Area Box Number of Averaged value on 01.01.2000
No. data (mBq/L)
Box Area ± 1σ
North Pacific 1 3 1.3 1.4 ± 0.2
2 31 1.6
3 3 1.4
4 13 1.5
5 5 1.1
Equatorial Pacific 6 2 1.5 1.3 ± 0.3
7 3 1.1
South Pacific 8 1 1.2 0.8 ± 0.3
9 4 1.1
10 3 0.8
11 4 0.6
12 2 0.4
Antarctic 13 1 0.1 0.1
Sea of Japan 14 42 1.6 1.6 ± 0.3
Arabian Sea 15 15 1.0 1.0 ± 0.2
Indian Ocean 16 7 1.1 1.1 ± 0.2
Southern Ocean 17 12 0.7 0.7 ± 0.4
Arctic 18 1 2.3 2.3
19
Barents Sea 20 7 1.9 1.9 ± 0.4
Baltic Sea 21 71 11.1 11.1 ± 2.9
North Sea 22 118 4.0 4.0 ± 1.2
Irish Sea 23 14 49 49 ± 83
English Channel 24 43 4.1 4.1 ± 1.4
North N. Atlantic 25 17 2.1 2.1 ± 0.9
Black Sea 26 15 17 17 ± 6
Mediterranean Sea 27 15 1.7 1.7 ± 0.2
North Atlantic 28 17 1.2 1.2 ± 0.6
Central Atlantic 29 5 0.8 0.8 ± 0.1
South Atlantic 30 2 0.4 0.4 ± 0.2

Normal Font: Standard deviation for area-averaged value

Italic Font: Standard deviation for box-averaged value

139
TABLE XX. 137Cs IN SURFACE WATER OF THE WORLD'S OCEANS AND SEAS

Area Box Number of Averaged value on 01.01.2000

No. data (mBq/L)
Box Area ± 1σ
North Pacific 1 4 2.0 2.4 ± 0.3
2 30 2.4
3 3 2.8
4 7 2.4
5 4 2.3
Equatorial Pacific 6 2 2.3 2.1 ± 0.3
7 3 1.9
South Pacific 8 1 1.7 1.3 ± 0.5
9 4 1.7
10 3 1.4
11 4 1.1
12 2 0.6
Antarctic 13 1 0.1 0.1
Sea of Japan 14 44 2.8 2.8 ± 0.5
Arabian Sea 15 17 1.6 1.6 ± 0.3
Indian Ocean 16 7 2.1 2.1 ± 0.3
Southern Ocean 17 12 1.0 1.0 ± 0.6
Arctic Ocean 18 1 14 14
19
Barents Sea 20 9 3.6 3.6 ± 2.0
Baltic Sea 21 214 61 61 ± 19
North Sea 22 144 6.7 6.7 ± 2.9
Irish Sea 23 28 57 57 ± 55
English Channel 24 44 4.2 4.2 ± 1.5
North N. Atlantic 25 15 4.2 4.2 ± 2.7
Black Sea 26 20 25 25 ± 3
Mediterranean Sea 27 18 2.6 2.6 ± 0.4
North Atlantic 28 16 1.7 1.7 ± 0.8
Central Atlantic 29 5 1.4 1.4 ± 0.2
South Atlantic 30 2 0.6 0.6 ± 0.1

Normal Font: Standard deviation for area-averaged value

Italic Font: Standard deviation for box-averaged value

140
TABLE XXI. 239,240Pu IN SURFACE WATER OF THE WORLD'S OCEANS AND
SEAS

Area Box Number of Averaged value on 01.01.2000

No. data (μBq/L)
Box Area ± 1σ
North Pacific 1 2 7.9 3.3 ± 2.8
2 6 3.8
3 3 0.7
4 7 2.4
5 2 1.7
Equatorial Pacific 6 5 3.6 3.1 ± 0.7
7 3 2.7
South Pacific 8 5 1.5 2.8 ± 2.1
9 4 5.7
10 2 4.3
11 4 1.6
12 1 0.8
Antarctic 13 1 1.3 1.3 ± 0.7
Sea of Japan 14 30 6.6 6.6 ± 2.5
Arabian Sea 15 13 1.9 1.9 ± 1.2
Indian Ocean 16 4 3.0 3.0 ± 1.5
Southern Ocean 17 10 1.0 1.0 ± 0.5
Arctic 18 24 6.4 6.4 ± 1.5
19
Barents Sea 20 7 20 20 ± 12
Baltic Sea 21 29 3.4 3.4 ± 2.5
North Sea 22 33 15 15 ± 10
Irish Sea 23 30 500 500 ± 400
English Channel 24 18 13 13 ± 8
North N. Atlantic 25 9 36 36 ± 16
Black Sea 26 5 5.3 5.3 ± 2.3
Mediterranean Sea 27 7 14 14 ± 4
N. Atlantic 28 17 5.0 5±3
C. Atlantic 29 5 2.8 2.8 ± 1.3
S. Atlantic 30 1 1.8 1.8 ± 0.6

Normal Font: Standard deviation for area-averaged value

Italic Font: Standard deviation for box-averaged value
Italic + Underline: Analytical error only

141
 90 137 239,240
TABLE XXII. MEAN RESIDENCE TIME OF Sr, Cs AND Pu IN SURFACE
WATER
Mean residence time ± 1σ *
(year)
90 137 239,240
Area Boxes Sr Cs Pu
North Pacific 1-5 17.9 ± 1.6 18.4 ± 2.0 9.7 ± 1.3
Equatorial Pacific 6+7 30.5 ± 2.7 41.3 ± 4.4 14.7 ± 3.4
South Pacific 8-12 25.8 ± 1.4 32.0 ± 7.5 17.5 ± 5.2
All Pacific 1-12 23.0 ± 3.5 22.9 ± 6.2 10.7 ± 1.6
North Indian 15 29.2 ± 2.7 30.6 ± 11.0
South Indian 16+17 31.6 ± 9.2 12.7 ± 1.5
All Indian 15-17 29.4 ± 2.6 13.0 ± 2.4
North Atlantic 25+28 22.6 ± 6.2 26.9 ± 6.0 13.0 ± 0.8
Central Atlantic 29 34.9 ± 3.0 34.3 ± 8.2 14.1 ± 4.2
South Atlantic 30 25.0 ± 12.7 29.2 ± 9.1 15.4 ± 7.1
All Atlantic 25-30 32.2 ± 3.5 29.4 ± 4.3 13.1 ± 0.8

All Oceans 27.5 ± 4.6 28.6 ± 2.1 12.7 ± 1.4

* Error weighted averaged values

Generally, as expected, the differences between the effective residence times of 90Sr and
137
Cs are, within uncertainties, the same. Longer residence times can be seen in both the
central Pacific and the central Atlantic Oceans. The mean residence time calculated for the
world ocean is 28 ± 3 years for 90Sr and 137Cs, and 13 ± 1 year for 239,240Pu.
Changes in radionuclide concentrations in water profiles with time in the N Atlantic and
Pacific Oceans were also studied. A clear decrease of radionuclide concentrations in surface
water was observed due to transport of radionuclides to medium water depths.
The results obtained in the framework of the WOMARS CRP provide the most
complete data set available to Member States on levels of anthropogenic radionuclides in the
marine environment. The results will be used as the international reference source on the
average levels of anthropogenic radionuclides in the marine environment, so that any further
contributions from nuclear reprocessing plants, radioactive waste dumping sites, nuclear
bomb test sites and possible nuclear accidents can be identified.

142
 ACKNOWLEDGEMENTS

This project would not have been possible without the generous support of the
Government of Japan, provided through its Science and Technology Agency. Therefore, it is a
great pleasure to acknowledge the collaboration between the IAEA's Marine Environment
Laboratory in Monaco and the Science and Technology Agency of Japan (presently the
Ministry of Education, Culture, Sports, Science and Technology — MEXT). The support
provided by the Governments of France, Germany, India, Italy, Japan and the Russian
Federation for IAEA-MEL's participation in international expeditions is also highly
acknowledged.

The major donors of data for the project were Japanese institutions, principally the
Japan Chemical Analysis Centre (JCAC), the National Institute of Radiological Sciences
(NIRS), the Marine Safety Agency (MSA) and the Fisheries Agency (FA). The IAEA would
like to thank T. Morimoto and T. Hashimoto of JCAC for their help with the transfer of data
from the JCAC database to the IAEA GLOMARD database. Data used for surface water
radionuclide time series in the Pacific Ocean were based on the HAM database developed in
the Geochemical Research Department of the Japan Meteorological Agency.

Further, the main data sets used in the project were kindly provided by the participating
institutions: The Federal Maritime and Hydrographic Agency (Germany), Risö National
Laboratory (Denmark), Japan Atomic Energy Research Institute, Marine Research
Laboratory, Mutsu Establishment (Japan), Japan Marine Science Foundation, Mutsu Marine
Laboratory (Japan), Korean Ocean Research Institute (Republic of Korea), Lawrence
Livermore National Laboratory (USA), Woods Hole Oceanographic Institute (USA) and
many other institutes (e.g. The Centre for Environment, Fisheries and Aquaculture Science,
(UK), The Institute of Radioprotection and Nuclear Safety (France)) as well as researchers.

It is a great pleasure to acknowledge the institutes and researchers who contributed to

this project by organizing oceanographic expeditions in which IAEA-MEL staff participated,
for example, the Joint Japanese-Korean-Russian expert groups, 1994 and 1995; the Federal
Fisheries Research Centre (Germany), 1996, 1998 and 2000; the Physical Research
Laboratory (India), 1998; the Marine Environment Research Centre, La Spezia (Italy), 1998
and the Centre National de Recherche Scientifique (France), 1999.

The fruitful collaboration with J.-F. Comanducci, J. Gastaud, C. Gustavsen, L. Huynh-

Ngoc, J. La Rosa, S.-H. Lee, I. Levy, L. Liong Wee Kwong, S. Mulsow, M. Nakano, B.
Oregioni, I. Osvath, M.K. Pham, H. Pettersson, H. Ramadan, P. Scotto, E. Wyse (IAEA-
MEL) as well as with researchers from many institutes who took part in analytical work
(W.E. Kieser and colleagues of The Canadian Centre for Accelerator Mass Spectrometry at
the University of Toronto (Canada); H. Nies and colleagues of the Federal Maritime and
Hydrographic Agency (Germany); B.L.K. Somayajulu and colleagues of the Physical
Research Laboratory (India); R. Delfanti and colleagues of the Marine Environment Research
Centre La Spezia (Italy); T. Aramaki and colleagues of the Japan Atomic Energy Research
Institute's Mutsu Marine Laboratory, K. Hirose and colleagues of the Meteorological
Research Institute of Japan, Y. Ikeuchi and colleagues of the Japan Chemical Analysis Center,
Sh. Shima and colleagues of the Mutsu Marine Laboratory of the Japan Marine Science
Foundation; G. Hoon Hong and colleagues of the Korea Ocean Research and Development
Institute (Korea, Rep. of); U. Morgenstern and colleagues of the Institute of Geological and
Nuclear Sciences (NZ); T. Jull and colleagues of the University of Arizona, Z. Top and
colleagues of the University of Miami (USA)) is highly acknowledged.

143
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152
 ANNEX I. TRANSFER COEFFICIENTS FOR 90Sr AND 137Cs FOR
DOSE CALCULATIONS

I-1. Introduction:

In the MARDOS report [3] an attempt was made to calculate the collective effective
doses from ingestion of marine products contaminated by 137Cs. In this Annex, the most
recent information on input of 90Sr and 137Cs to the world ocean has been used. Transfer
factors between input and collective effective dose have been calculated for the terrestrial and
the marine environment. Table I shows the calculation of the ingestion doses from marine
foods (fish and shellfish, i.e. crustaceans and molluscs).

I-2. Input:

It has been assumed that all input of 137Cs (and 90Sr) from reprocessing and the
Chernobyl accident occurred in the North Atlantic and Arctic Oceans and that these parts of
the world ocean still contain this activity (or the rest after decay). Most of the activity is
probably still present in the 90-60ºN latitude band rather than in the 90-30ºN band. Hence,
one may have underestimated the radiological impact from these two sources, as the fish catch
is high in the 90-60ºN belt.

I-3. Volume:

The mixed layer of the ocean is assumed to be presented by the upper 100 m water
layer. Hence, the volume of the mixed layer is obtained by multiplying the area (given in m2)
by 100.

I-4. Catch:

The fishing areas used in the FAO statistics do not strictly follow the division used here.
Therefore, it has been necessary to make some adjustments. The catch in areas 71 and 77 in
the Pacific have been totalled and divided by two; one half has been allocated to 30-0ºN and
the other to 0-30ºS. In the Indian Ocean the three areas: 51, 57 and 58 have been added
together and the total catch has been divided between the latitude bands 30-0ºN, 0-30ºS and
30-90ºS, proportional to the area of these latitude bands for the Indian Ocean (i.e. 16%, 36%
and 48%, respectively).

The catch data are the FAO’s 1990 data used in the MARDOS report [3]. The doses
may be overestimated because the catch has increased over the years, whereas the
concentrations for 90Sr and 137Cs have decreased.

I-5. Concentrations in fish and shellfish:

The 137Cs concentrations in fish and shellfish were obtained by multiplying the water
concentration by 100 and 30, respectively [3].

I-6. Time integral:

It has been assumed that the mean residence time for 137Cs (and 90Sr) in the mixed layer
of the ocean is 25 years. Time integrals were thus calculated by multiplying the
concentrations by 25. If the mean residence times of 90Sr and 137Cs are shorter in the N

153
Atlantic Ocean as indicated by observations in the Faroes and Greenland, the doses from the
North Atlantic are overestimated by approximately one third.

I-7. Dose calculation:

137
The collective effective dose was calculated by multiplying the sum of the Cs
inventories in the fish and shellfish catch by 1.25·10-8 Sv/Bq.

Table II shows the calculation of transfer coefficients.

The transfer coefficient (manSv/PBq) for 90Sr in global fallout was calculated from the
transfer coefficient for 137Cs taking into account that the dose factor for 90Sr (ingestion) is
2.8/1.3 = 2.15 times higher than that of 137Cs, whereas the marine concentration factor
(consumption weighted) is 44 times higher for 137Cs than for 90Sr (fish and shellfish) [3].
Hence, the manSv/PBq transfer coefficient for 90Sr becomes (2.15/44)*15 = 0.73. For global
fallout the terrestrial dose consists for 137Cs of 64% external radiation and 36% ingestion. For
90
Sr, 92% comes from ingestion and 8% from inhalation.

I-8. Chernobyl

In the UNSCEAR report [2], exposures and effects of the Chernobyl accident are
reported. This Annex deals preliminarily with the situation in the most contaminated areas of
the FSU, i.e. areas that have received more than 37 kBq 137Cs m-2 from the accident. The total
collective effective doses to the population in these areas are 40300 manSv from external
exposure and 20400 manSv from ingestion (thyroid doses are not included). The ingestion
dose comes essentially from 137Cs, 134Cs and 90Sr. UNSCEAR [2] estimates that the 90Sr
contribution to the effective dose from internal exposure does not exceed 5–10%, i.e. ~
1500 manSv. The releases from the Chernobyl accident were ~10 PBq 90Sr, ~54 PBq 134Cs
and ~85 PBq 137Cs. The amount of 137Cs deposited in the contaminated areas (>37 kBq
137
Cs m-2) of the FSU was 29 PBq, the amounts of 134Cs and 90Sr were 18 PBq and 10 PBq,
respectively. The transfer coefficient from input to collective dose for 90Sr is calculated to be
1500/10 = 150 manSv/PBq for the Chernobyl accident. In order to calculate the corresponding
transfer coefficient for 137Cs one has to correct for the 134Cs contribution to the effective
doses. In the case of external exposure the ratio between the collective doses from the same
inputs of 137Cs and 134Cs is 5.372 and for ingestion the ratio is 1.44. Hence, the ratio between
the external 137Cs and 134Cs Chernobyl dose becomes (29/18)*5.372 = 8.6549, and for the
ingestion dose the ratio becomes (29/18)*1.44 = 2.32. The external collective effective dose
for 137Cs then becomes

8.6549
40300 = 36125 manSv and the corresponding dose from ingestion:
9.6549
2.32
(20400-1500) = 13207 manSv.
3.32
The total dose from the 29 PBq 137Cs becomes 49333 manSv and the transfer coefficient for
137 49333
Cs is calculated to be = 1700 manSv/PBq. The total terrestrial deposition of 137Cs
29
was 85-16 = 69 PBq and if one assumes the same transfer factor valid for the remaining part
of the terrestrial environment as found for the FSU, the collective effective dose from 69 PBq
137
Cs is calculated to 69*1700 = 117400 manSv. This figure is about 3 times less than earlier
estimates.

154
 The collective effective dose from Chernobyl released to the marine environment was
calculated by applying a weighted transfer coefficient: 0.75*98+0.25*15 = 77 manSv/PBq
137
Cs. The assumption was that 75% of the debris went to coastal water and 25% to the open
sea. For coastal water the transfer coefficient (98 manSv/PBq 137Cs) used for reprocessing
discharges was applied and for the open sea the transfer coefficient applied for global fallout
was used.

I-9. Reprocessing

UNSCEAR has calculated the transfer coefficient for releases of 90Sr and 137Cs into
coastal water to be 4.7 manSv/PBq 90Sr and 98 manSv/PBq 137Cs. These figures have been
used together with the release data of the two radionuclides from Sellafield and Cap de la
Hague in the calculation of the collective effective doses from water-borne discharges from
nuclear reprocessing.

I-10. Comparison between transfer coefficients

If all sources are considered, Table II shows that the terrestrial pathway for 137Cs
(ingestion and external radiation) has a 6928/22 ≈ 300 times higher transfer coefficient than
the marine pathway. For 90Sr, the ratio between the two pathways is even higher namely
2634/0.80 ≈ 3000. If one considers global fallout and ingestion only, the ratio for 137Cs
8100 * 0.36 2740 * 0.92
becomes ≈ 200 and for 90Sr it is ≈ 3000. Discharges in coastal seas,
15 0.73
as has been seen from nuclear reprocessing, show a higher marine transfer coefficient than
global fallout.

155
 TABLE I. INGESTION DOSES FROM MARINE FOODS

156
Atlantic and Arctic Oceans Pacific and Indian Oceans World

90-30°N 30- 0-30°S 30-90°S 90 N- 90- 30-0°N 0-30°S 30-9°S 90N-

0°N 90°S 30°N 90°S
Input source
137
Global fallout Cs PBq 115.4 49.3 16.5 27.3 208.5 116.7 126.6 66 85.5 394.8 603.3
137
Reprocessing Cs PBq 40 40 40
137
Chernobyl Cs PBq 16 16 16
137
Total Cs PBq 171.4 49.3 16.5 27.3 264.5 116.7 126.6 66 85.5 394.8 659.3

Annual catch Fish (t/year) 1117555 503861 1466179 146617 191465 471845 463481 5705171 479905 1985749 9004020
7 0 9 25 5 0 9 5
Shellfish 2394607 732627 511030 511031 414929 531600 707820 855427 641662 7520910 1670205
(t/year) 5 1

Mixed ocean layer

Area 1012 m2 37.28 23.493 19.145 26.604 106.522 26.725 67.147 78.807 81.909 254.588 361.11
15 3
Volume 10 m 3.728 2.3493 1.9145 2.6604 10.6522 2.6725 6.7147 7.8807 8.1909 25.4588 36.111
137
Conc. in water Cs Bq/m3 45.97639 20.9849 8.618438 10.2616 85.8414 43.6669 18.8541 8.374890 10.4384 81.33443 167.1759
5 74 2 15 22 78 56 6 13 8
137
Time integral in water Cs 1149.409 524.624 215.4609 256.540 2146.03 1091.67 471.353 209.3722 260.960 2033.361 4179.397
(Bq/m3) y 9 36 6 37 56 45 9 6 33
137
Conc. in fish Cs Bq/t 4597.639 2098.49 861.8438 1026.16 8584.14 4366.69 1885.41 837.4890 1043.84 8133.443 16717.59
5 74 2 15 22 78 56 6 13 8
137
Conc. in shellfish Cs Bq/t 1379.291 629.549 258.5531 307.848 2575.24 1310.00 565.624 251.2467 313.152 2440.033 5015.276
8 23 5 44 27 94 67 2 4 1
137
Time integral in fish Cs (Bq/t) 114940.9 52462.4 21546.09 25654.0 214603. 109167. 47135.3 20937.22 26096.0 203336.1 417939.7
y 9 36 6 37 56 45 9 6 33
137
Time integral in Cs (Bq/t) 34482.29 15738.7 6463.828 7696.21 64381.0 32750.2 14140.6 6281.167 7828.81 61000.82 125381.9
shellfish y 6 31 7 11 67 34 17 9 9
 Inventory in fish catch TBq 1.284529 0.26433 0.031590 0.03761 1.61807 0.51510 0.21846 0.119450 0.12523 0.978252 2.596323
6 78 4 34 11 17 36 5 64 1
Inventory in shell fish TBq 0.082571 0.01153 0.003303 0.00393 0.10133 0.17410 0.01000 0.005373 0.00502 0.194505 0.29584
catch 5 06 2 3 84 03 9 1 34 8 42

Dose calculation
Intake by fish TBq 0.449585 0.09251 0.011056 0.01316 0.56632 0.18028 0.07646 0.041807 0.04383 0.342388 9087131
consumption 3 82 7 47 49 56 23 7 27 2
Intake by shellfish TBq 0.041285 0.00576 0.001651 0.00196 0.05066 0.08705 0.00500 0.002686 0.00251 0.097252 1479221
consumption 8 53 6 65 92 01 45 5 17 9
Collective effective ManSv 6136 1229 159 189 7712 3342 1018 556 579 5496 13208
dose

157
 TABLE II. CALCULATION OF COLLECTIVE EFFECTIVE DOSES FOR MARINE AND TERRESTRIAL PATHWAYS

158
(WORLD POPULATION: 5.6*109)
Source
Pathway Release in PBq manSv/PBq (manSv)*103 References
Sr-90 Cs-137 Sr-90 Cs-137 Sr-90 Cs-137
________________ _ _______ _______ __ _______ __ _______ __ _______ __ _______ __ _______ __ _________________
Global fallout marine 377 a,c 603 a,c 0.73 c 15 c 0.28 c 9.1 c a) UNSCEAR [2]
terrestrial 235 a,c 316 a,c 2740 a,c 8100 a,c 643.9 a,c 2550.0 a,c c) WOMARS
(this work)
Nuclear reprocessing marine 6.6 A 39.7 a 4.7 a 98 a 0.03 c 3.9 a
terrestrial 0 C 0 c 0 0

Chernobyl accident marine 0 C 16 c 3.7 77 c 0 c 1.2 c

terrestrial 10 A 69 a,c 150 a,c 1700 a,c 1.50 a,c 117.3 a,c

Total marine 383.6 658.7 0.80 22 0.31 14.2

terrestrial 245 385 2634 6928 645.40 2667.3

Sum 629 1043.7 1027 2569 646 2681.5

 ANNEX II. LIST OF PUBLICATIONS PUBLISHED BY THE IAEA-MEL/RML
STAFF ON WORLDWIDE MARINE RADIOACTIVITY STUDIES

1. Povinec P.P., Togawa O.: Worldwide Marine Radioactivity Studies - Assessing the Picture,
IAEA Bulletin, 40 (1998) 11-17.

2. Hirose K., Amano H., Baxter M.S., Chaykovskaya E., Chumichev V.B., Hong G.H., Isogai
K., Kim C.K., Kim S.H., Miyao T., Morimoto T., Nikitin A., Oda K., Pettersson H.B.L.,
Povinec P.P., Seto Y., Tkalin A., Togawa O., Veletova N.K.: Anthropogenic Radionuclides in
Seawater in the East Sea/Japan Sea: Results of the First-Stage Japanese-Korean-Russian
Expedition, Journal of Environmental Radioactivity, 43 (1999) 1-13.

3. Ikeuchi Y., Amano H., Aoyama M., Berezhnov V.I., Chaykovskaya E., Chumichev V.B.,
Chung C.S., Gastaud J., Hirose K., Hong G.H., Kim C.K., Kim S.H., Miyao T., Morimoto T.,
Nikitin A., Oda K., Pettersson H.B.L., Povinec P.P., Tkalin A., Togawa O., Veletova N.K.:
Anthropogenic Radionuclides in Seawater of the Far Eastern Seas, The Science of the Total
Environment, 237/238 (1999) 203-212

4. Jull A.J.T., Burr G.S., Courtney C., Povinec P.P., Togawa O.: Measurements of
Radiocarbon in the NW Pacific Ocean and its Marginal Seas, IAEA-TECDOC-1094, Vienna,
1999, pp.249-253

5. Pettersson H.B.L., Amano H., Bereznhov V.I., Chaykovskaya E., Chumichev V.B., Chung
C.S., Gastaud J., Hirose K., Hong G.H., Kim C.K., Kim S.H., Lee S.H., Morimoto T., Nikitin
A., Oda K., Povinec P.P., Suzuki E., Tkalin A., Togawa O., Veletova N.K., Volkov Y.,
Yoshida K.: Anthropogenic Radionuclides in Sediments in the NW Pacific Ocean and its
Marginal Seas: Results of the 1994-1995 Japanese-Korean-Russian Expeditions, The Science
of the Total Environment, 237/238 (1999) 213-224.

6. Povinec P.P., Huynh-Ngoc L., Liong Wee Kwong L., Mulsow S., Oregioni B., Togawa O.,
Goroncy I., Uhde H.H., Rengarajan R., Hirose K., Ikeuchi Y., Ito T., Shima S., Fukasawa M.,
Moriya H., Kazama T., Ozawa S., So A.., Yasuzumi S., Lee S.H., Park S.K., Pettersson
H.B.L.: The IAEA ’97 Pacific Ocean Expedition, , IAEA-TECDOC-1094, Vienna, 1999,
pp.399-400.

7. Povinec P.P., Togawa O.: Marine Radioactivity Studies in the World Oceans (MARS),
IAEA-TECDOC-1094, Vienna, 1999, pp.262-267.

8. Povinec P.P., Gayol J., Togawa O.: Global Marine Radioactivity Database (GLOMARD),
IAEA-TECDOC-1094, Vienna, 1999, pp.481-482.

9. Togawa O., Povinec P.P., Pettersson H.B.L.: Collective Dose Estimate by the Marine Food
Pathway from Liquid Radioactive Wastes Dumped in the Sea of Japan, The Science of the
Total Environment, 237/238 (1999) 241-248.

10. Cetina M., Rajar R., Povinec P.P.: Modelling of Circulation and Dispersion of
Radioactive Pollutants in the Japan Sea, Oceanologica Acta, 23 (2000) 819-836.

11. Livingston H.D., Povinec P.P.: Anthropogenic Marine Radioactivity, Ocean & Coastal
Management, 43 (2000) 689-712.

159
12. Povinec P.P., Oregioni B., Jull A.J.T., Kieser W.E., Zhao X.-L.: AMS Measurements of
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C and 129I in Seawater Around Radioactive Waste Dump Sites, Nuclear Instruments and
Methods in Physics Research, B 172 (2000) 672-678.

13. Aoyama M., Hirose K., Miyao T., Igarashi Y., Povinec P.P.: Temporal Variation of 137Cs
Inventory in the Western North Pacific, Journal of Radioanalytical & Nuclear Chemistry, 248
(3) (2001) 785-787.

14. Aoyama M., Hirose K., Miyao T., Igarashi Y., Povinec P.P.: 137Cs Activity in Surface
Water in the Western North Pacific, Journal of Radioanalytical & Nuclear Chemistry, 248 (3)
(2001) 789-793.

15. Aramaki T., Mizushima T., Kuji T., Povinec P.P., Togawa O.: Distribution of
Radiocarbon in the Southwestern North Pacific, Radiocarbon, 43 (2B) (2001) 879-886.

16. Kershaw P.J., Livingston H.D., Povinec P.P., Heldal H.E.: Contrasting Behaviour of
Artificial Radionuclides in the Pacific and Other Ocean Basins: Radionuclides as Tracers of
Environmental Change. Environmental Changes and Radioactive Tracers, (2002) 436-447.

17. Livingston H.D., Povinec P.P., Toshimichi I., Togawa O.: The Behaviour of Plutonium in
the Pacific Ocean, in Plutonium in the Environment, Env. Radiact. Ser. 1 (2001) 267-292.

18. Livingston H.D., Povinec P.P.: A Millenium Perspective on the Contribution of Bomb
Fallout Radionuclides to Ocean Science, Health Physics, 82 (5) (2002) 656-668.

19. Povinec P.P., Jull A.J.T., Burr G.S.: Radiocarbon in Seawater at Radioactive Waste
Dumping Sites in the NE Atlantic and NW Pacific, Radiocarbon, 43 (2B) (2001) 879-886.

20. Povinec, P.P., Livingston, H.D., Shima, S., Fifield, K., Gastaud, J., Goroncy, I., Hirose,
K., Ikeuchi, Y., Ito, T., Liong Wee Kwong, L., Lee, S-H., Moriya, H., Mulsow, S., Oregioni,
B., Togawa, O., Wyse, E.: IAEA'97 Expedition to the NW Pacific Ocean –Results of
Oceanographic and Radionuclide Investigations of the Water Column, Deep-Sea Research II,
50 (2003) 2607.

21. Hirose, K., Aoyama, M., Povinec, P.P.: Particulate Plutonium in Seawater of the Western
North Pacific: Its Concentrations in Surface and Deep Waters, Deep-Sea Research II, 50
(2003) 2639.

22. Moon, D-S., Hong, G-H., Kim, Y.I., Baskaran, M., Chung, C.S., Kim, S-H., Lee, H-J.,
Lee, S-H., Povinec, P.P.: Accumulation of Artificial and Natural Radionuclides in the Bottom
Sediments of the Northwest Pacific Ocean, Deep-Sea Research II, 50 (2003) 649.

23. Ito, T., Povinec, P.P., Togawa, O., Hirose, K.: Temporal and Spatial Variations of
Anthropogenic Radionuclides in the Japan Sea Water, Deep-Sea Research II, 50 (2003) 2701.

24. Lee, S-H., Chung, C-S., Gastaud, J., Hong, G-H., Kim, S-H., Lee, K-W., Pettersson,
H.B.L., Povinec, P.P.: Investigation of Plutonium and Americium in the Marginal Seas of the
Northwest Pacific Ocean, Deep-Sea Research II, 50 (2003) 2727.

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25. Povinec, P.P., Delfanti, R., Gastaud, J., La Rosa, J.J., Morgenstern, U., Oregioni, B.,
Pham, M.K., Salvi, S., Top, Z.: Anthropogenic Radionuclides in Indian Ocean Surface Waters
–the Indian Ocean Transect 1998, Deep-Sea Research II, 50 (2003) 2751.

26. Mulsow, S., Povinec, P.P., Somayajulu, B.L.K., Oregioni, B., Liong Wee Kwong, L.,
Gastaud, J., Top, Z., Morgenstern, U.: Temporal and Spatial Variations of 3H, 90Sr, 239,240Pu
and 241Am in the Arabian Sea: GEOSECS Stations revisited, Deep-Sea Research II, 50 (2003)
2761.

27. Bhushan, R., Dutta, K., Mulsow, S., Povinec, P.P., Somayajulu, B.L.K.: Distribution of
Natural and Man-made Radionuclides during Reoccupation of GEOSECS Stations 413 and
416 in the Arabian Sea: Temporal Changes, Deep-Sea Research II, 50 (2003) 2777.

28. Povinec, P.P., Bailly du Bois, P., Kershaw, P.J., Nies, H.: Temporal and Spatial Trends in
the Distribution of 137Cs in Surface Waters of Northern European Seas –a Record of 40 Years
of Investigations, Deep-Sea Research II, 50 (2003) 2785.

29. Nakano, M., Povinec, P.P.: Oceanic General Circulation Model for the Assessment of the
Distribution of 137Cs in the World Ocean, Deep-Sea Research II, 50 (2003) 2803.

30. Lee, S-H., La Rosa, J.J., Levy-Palombo, I., Pham, M.K., Povinec, P.P.: Recent Input of
137
Cs, 239,240Pu and 241Am to the Northwest Mediterranean Sea, Deep-Sea Research II, 50
(2003) 2817.

31. Povinec, P.P., Froehlich, K., Gastaud, J., Oregioni, B., Pagava, S.V., Pham, M.K.,
Rusetski, V.: 90Sr, 137Cs and 239,240Pu in the Caspian Sea –a Contribution to Water Dynamics
Studies, Deep-Sea Research II, 50 (2003) 2835.

32. Nakano, M., Povinec, P.P.: Modelling the Distribution of Plutonium in the Pacific Ocean,
Journal of Environmental Radioactivity, 69 (2003) 85.

161
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 PARTICIPANTS IN THE COORDINATED RESEARCH PROJECT

Aarkrog, A. Risø National Laboratory,

P.O. Box 49, DK-4000 Roskilde, Denmark

Buesseler, K.O. Department of Marine Chemistry and Geochemistry,

Woods Hole Oceanographic Institution,
Clark 447 WHOI, Woods Hole, MA 02543,
United States of America

Delfanti, R. ENEA,
Marine Environment Research Centre,
C.P. 316, I-19100 La Spezia, Italy

Hirose, K. Geochemical Research Department,

Meteorological Research Institute,
Japan Meteorological Agency,
1-1 Nagamine, Tsukuba-shi,
Ibaraki-ken 305-0052, Japan

Hoon Hong, Gi Isotope Oceanography,

Korea Ocean Research & Development Institute,
Ansan P.O. Box 29, Seoul - 425-600, Republic of Korea

Ito, T. IAEA Marine Environment Laboratory, Monaco,

4 Quai Antoine 1er,
MC-98000 Monaco

Livingston, H.D. IAEA Marine Environment Laboratory, Monaco,

4 Quai Antoine 1er,
MC-98000 Monaco

Nies, H. Federal Maritime and Hydrographic Agency,

Marine Chemistry/Laboratory Suelldorf,
Bernhard-Nocht-Str. 78, 20359 Hamburg, Germany

Noshkin, V.E. Lawrence Livermore National Laboratory,

University of California,
7000 East Avenue, P.O. Box 808,
Livermore CA 94550, United States of America

Povinec, P.P. IAEA Marine Environment Laboratory, Monaco,

4 Quai Antoine 1er,
MC-98000 Monaco

Shima, Sh. Mutsu Marine Laboratory,

Japan Marine Science Foundation,
4-24 Minato-machi, Mutsu-shi, Aomori-ken 035-0064, Japan

Togawa, O. IAEA Marine Environment Laboratory, Monaco,

4 Quai Antoine 1er,
MC-98000 Monaco

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