LBL--15685

DE83 006967
NUCLEAR REACTIONS AND SYNTHESIS OF NEW TRANSURANIUM SPECIES

Glenn T. Seaborg

This paper is to be presented at a Workshop on Future Directions in

Transplutonium Elenent Research in Washington, D. C., February 28 -

March 2, 1983.

January 1983

Nuclear Sciences Division

Lawrence Berkeley Laboratory
University of California
Berkeley, CA 94720

This work was supported by the Director, Office of Energy Research,

Division of Nuclear Physics of the Office of High Energy and Nuclear Physics

of the U. S. Department of Energy under Contract DE-AC03-76SF00098.

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CONTRIBUTION TO WORKSHOP ON FUTURE DIRECTIONS IN TRANSPLUTONIUM ELEMENT RESEARCH

Washington, D. C , February 28 - March 2, 1983

NUCLEAR REACTIONS AND SYNTHESIS OF NEW TRANSURANIUM SPECIES

By Glenn T. Seaborg

At the time of this writing (late 1982) 16 transuranium elements are known

(atomic numbers 93 to 107, inclusive, and number 109). Distri ted among these

16 elements are nearly 200 nuclear species. Those with atomic numbers 93 to 101,

inclusive, were first synthesized and identified (i.e., discovert!) through the

use of neutrons, deuterons or helium ions. The half lives become shorter and

shorter with increasing atomic number, until at elements 107 and 1(P theae are

in the range of milliseconds.

Three of the transuranium elements (numbers 104, 105 and 106) a:-! a large

proportion of the transfermium (beyond number 100) nuclear specie" discovered

during the last IS years have utilized actinide isotopes produced in the HFIR -

TRU facilities at ORNL as the target material. Present indications are that most

of the future discoveries of new transuranium nuclear species and the discovery

of superheavy elements, if successfully accomplished, will utilize such target

material.

In this short review, I shall describe the special aspects of heavy ion

nuclear reaction mechanisms operative in the transuranium region, the role of new

techniques, possible nuclear reactions for the production of additional trans­

uranium elements and nuclear species and the importance of work in this region

for the development of nuclear models and theoretical concepts. This discussion

should make it clear that a continuing supply of elements and isotopes, some of

them relatively short-lived, produced by the HFIR-TRU facilities, will be a

requirement for future synthesis of new elements and isotopes.

 - 2

In this short account, I shall not cover the historical aspects except for

s o w brief references that are indispensable to an understanding of the these.

A compilation of reprints of the original publications, accompanied by explana­

tory material, covers very thoroughly all aspects of the historical background of

the transuranium elements through atomic number 106. This includes such infor­

mation on the discovery of these elements, including accounts of the competing

claims for the discovery of elements 104, 105 and 106 by scientists at the Dubna

Laboratory in the Soviet Union, as well as original information on many isotopes,

nuclear reactions for their production, radioactive properties, chemical properties

of the elements, etc. The discovery of all elements beycnd atomic number 100

(fermium) has been made on a one-atom-at-a-time basis and this will surely continue

to be the case. It has been crucial to the claim of discovery that the atomic

number of the reaction product be clearly identified using chemical or physical

techniques. Criteria for establishing that such an identification has been made
2
have been published by an international group of experts an<< these criteria will

guide the discussions in the review.

Nuclear stability considerations and radioactivity decay properties, which

are of central importance in devising experiments for the production and identi-
3
fication of new elements and new isotopes, are the subject of another paper

prepared for this workshop.

However, for the convenience of the reader, I shall briefly summarize some

salient information about superheavy elements (SHE). Simple extrapolations of

radioactive decay properties for elements beyond atomic number 109 suggest that

the half life, especially that for decay by spontaneous fission, shall become so

short as to make detection very difficult and soon impossible. However, in the

period from 1966 to 1972, a number of calculations based on modern theories of

nuclear structure showed that in the region of proton number Z - 114 and neutron
 - 3

number N » 184 the ground states of nuclei should be stabilized against decay by

spontaneous fission. This stabilization is due to the complete filling of major

proton-and nui.'tron-shells in this region and is analogous to the stabilization

of chemical elements such as the noble gases by the filling of their electronic

shells. Such superheavy elements are predicted to form an island of relative

stability extending both above and below Z - 114 and N - 184 and separated from

the peninsula of known nuclei by a sea of instability.

Some more recent calculations, based on careful consideration of the effect

of mass asymmetry on the fission barrier and a reduced spin-orbit coupling

strength, have indicated that the Z • 114 shell effect is not very large. These

calculations do confirm the exirf;nce of a shell at N - 184, but also suggest less

stability for species with N < 184; that is, the island of stability has a cliff

with a sharp drop-off for N < 184. If these considerations are correct, it would

become considerably more difficult to synthesize and detect the superheavy

elements. A premium would be placed on producing a nucleus with N " 184 or very

close to this, N • 183, in order that it might have a half life sufficiently long

to make it detectable.

During the last IS years numerous attempts have been made to synthesize and

identify superheavy elements through the bombardment of heavy target nuclei with

heavy ions. None of these experiments has been successful. A summary and

analysis suggests that this failure is not due to the failure to produce super­

heavy intermediate nuclei, but is due to the low survival probabilities of these

superheavy precursors.

NUCLEAR REACTION MECHANISMS

Nuclear reactions designed to produce isotopes in the transplutonium region

are dominated by the competing fission reaction, which diminishes the yield of
 - 4

the desired products. This diminution in yield is usually viry drastic and is

greater the higher the atomic number and degree of excitation of the inter­

mediate nucleus. The tendancy toward undergoing this unwanted fission also

increases with increasing angular momentum imparted to the intermediate nucleus.

(Angular momentum increases with th^ increasing mass of the bombarding projectile

nucleus and with the increasing magnitude of the impact parameter, the lateral

distance between the centers of the target and projectile nuclei). Thus, the

name of the game is to produce intermediate nuclei with a minimum of excitation

(cold nuclei) and a minimum of angular momentum so they can reach the ground state

(usually through the emission of neutrons and gamma-rays) with the minimum of loss

from the competing fission reaction.

There are a number of heavy ion reaction mechanisms that might lead to the

identification of new isotopes, and in one case possibly new elements, through the

production of cold nuclei in sufficient yields to be detectable. The compound

nucleus mechanism, known and understood for the longest time, offers the best, and

probably the only, hope for the production and identification of new elements; this

seems to be operable with heavy element target nuclei (lead and bismuth) only for

heavy ion projectiles with atomic number up to 26 (iron) - for transplutonium

targets, this limitation produces no roadblock to the possible production of

Superheavy Elements.

The other heavy ion nuclear reaction mechanisms cover a range of categories

whose definition is not always unambiguous and which tend to merge at the

boundaries of the definitions one into the other. An oversimplified categori­

zation into two types will serve our present purposes. One type is well described

as simple transfer reactions and is applicable for our purposes (transplutonium

targets) with light heavy ions - up to atomic number 10 (neon) or somewhat higher.

The other can be described as deep inelastic transfer reactions, whose importance
 - 5

increases with the increasing atomic number of the heavy ion projectile, with

uranium projectiles the most interesting for transplutonium targets.

Compound Nucleus Mechanism. This mechanism involves the complete amalga­

mation (complete fusion) of the heavy ion projectile with the target nucleus,

followed by the de-excitation of this compound nucleus through the emission

(usually) of neutrons and gamma-rays in competition with the more prevalent

fission reaction. The most central collisions (smallest impact parameter) which

impart only a small amount of angular momentum to the system, lead to such

complete fusion of the projectile and target nuclei. The product nuclei are

strongly focused in the forward (i.e., the projectile beam) direction due to

momentum conservation. The classical method of preparing transuranium nuclei has

been through the use of the complete fusion reaction. A typical example is the
2 I B
synthesis of element 106 by Ghiorso et al. who bombarded *'cf with 95 MeV 0
2 l 2 6 s
and observed the *'cf ( *0, 4n) 1 0 6 reaction with a cross section of V).3nb.
2 S 3
The 1 0 6 atoms (t^ * 0-9 ± 0.2 sec) were identified by observing the previously
2 s , 2 5 s
known daughter, R f , and granddaughter, N o , through the decay sequence
2 6 3 2 5 , 2 5 s 2 6 3
106 " Rf ° N o ° . The 1 0 6 atoms were isolated using a helium jet

and deposited on the rim of a wheel. The deposit was then rotated in front of a

sequence of surface barrier detectors which then detected the primary a-decay of
2 6 3
106. These primary detectors were then moved to face another series of second­

ary detectors which detected the decay of the previously known daughter atoms

implanted in the primary detectors by recoil in the initial decay. The time

correlated decay information was recorded using an on-line computer. A total of

14 time-correlated events was observed.

HoveveT, despite successes such as this, if we look at the cross sections

for complete fusion reactions such as the X (heavy ion, an) Y reaction, we find

a sharp decrease in the magnitude of these cross sections as the (Z,A) of the
 - 6

heavy ion projectile increases. As a further constraint, the limits on availa­

bility of target materials with Z > 98, presents great, but no insurmountable,

difficulties in synthesizing new transuranium nuclei with complete fusion

reactions. A number of workers, particularly those in the Soviet Union, have

pointed out that if some heavy ion projectiles with 40 K A < 60 are used in

combination with tightly bound target nuclei containing closed shells of nucleons,

it is possible to form extremely "cold" compound nuclei whose survival probabili­

ties might be high enough to compensate for the decreased complete fusion cross

sections.

A number of experimental studies involving the magic lead and bismuth nuclei

have shown that the possibility of such "cold fusion" reactions is, in fact, a

reality. Flerov et^ a^. observed the production of 2

No using the 2 D 6
Pb
25l,
('''Ca, 2n) reaction, while Nitschke «£ a_l. found N o to be produced with a
20
surprisingly large cross section of 3.4 ± 0.4 pb in the * P b (^'Ca, 2n) reaction.
2l
In this same manner, Gaggeler e_t aJL. observed the production of "'Fm in the
2 0 6
P b (""Ar, 2n) reaction.

The principal development, however, that has pushed "cold fusion" reactions

to the forefront in efforts to synthesize new transuranium nuclei was the work of
it ii 12

Munienberg e_£ jil. • using the velocity filter SHIP at GSI. They have observed
2 0 7 50 2 5 5 2 0 9
unambiguous evidence for the occurrence of the P b ( Ti, 2n) R f and Bi
50 2 5 7
( Ti, 2n) H a reactions at a bombarding energy of 4.85 MeV/u. Most interestingly
5 0 2 0 8 50 2 5 7
at a T i energy of 235 MeV (4.70 MeV/A), they observed the Pb ( Ti,n) Rf

reaction. Since SHIP is a velocity separator, "transfer" and "deep inelastic"

products are strongly suppressed since the products from these binary reactions

have a wide angular distribution and do not move with the velocity of the complete

fusion evaporation residues. The separator accepts recoils only from a limited

range of angles near 0° ; thut', these reactions are quite probably cold complete

fusion reactions.
 Of special interest is the use of cold fusion reactions to synthesize, and
11 13
2 0 9
thus discover, element 107 and element 109. For the former, B i was
!l, 2 0 s 2 6 2
bombarded with 4.85 and 4.95 MeV/u Cr and the B i ("Cr.n) 1 0 7 reaction

was observed. The identification of the 2 6 2

1 0 7 (t, • 4.7 , ms) was based upon

the observation of a set of correlated alpha particle decays which end in the
2 5 0
known F m decay. No complete decay chains were observed due to the small yield

and the 50Z efficiency of the detector system, but two partially complete chains
2 5 0 25l
ending in F m were observed and one chain ending in *Lr was observed. The
2 6 2
velocity of the 1 0 7 atoms was determined two different ways, by the velocity

separator itself and by a time-of-flight measurement. The energy of the evapora­

tion residue was measured and agreed with expectations for the cold fusion
13

mechanism. Similarly, element 109 was identified as the result of the bombard­
2 0 , 5 8 2 D , 5
ment of B i with 5.15 meV/u F e ions according to the reaction B i ( *Fe,n)
2 6 6 2 6 6
109. A single atom of 1 0 9 (which decayed after a time interval of 5 ms) was

identified through the observation of correlated alpha particle and spontaneous

fission decays involving previously known products.

Transfer Reactions. In this type of nuclear reaction there is transfer of

nucleons from the projectile to the target nucleus leading (of interest to us) to

products with atomic numbers all the way from that of the target nucleus to that

of the compound nucleus. (The transfer of just a couple of nucleons is also re­

ferred to as quasielastic scattering and the transfer of a large part of the

projectile is alternatively referred to as "massive transfer" or "incomplete

fusion"). These reactions seem to result from the more peripheral collisions

(those with larger impact parameters) and higher angular momentum. The product

nuclei are not so Btrongly focused in the forward direction as in the case of the

compound nucleus mechanism. For light heavy ions and heavy target nuclei, of

primary interest to us, the protons transfer preferentially from the projectile

nucleus to the target nucleus, a tendency that can be understood by considering

the potential energies of the systems near contact.
14

One of the first and more careful studies of these heavy ion "transfer"

reactions invoKlng production of transuranium nuclei was done by Hahn et al.

This remains one of the few studies in which kinematic measurements were attempted.

Hahn et £l. studied the excitation functions, recoil range distributions and

angular distributions of the heavy transuranium recoil products. In particular,

2 u ! 2l,l
they studied the characteristics of the production of C f and *Cf via the
2 3 , 12 2 3 9 I2
transfer reactions P u ( C, c2n) and P u ( C a3n) and via the complete
2 3 8 12 2 3 a 1 2
fusion reactions U ( C, 5n) and U( C , 6n). As expected, the complete

fusion reaction products are strongly forward focused with their angular distri­

bution peaked at 0 and show Gaussian range distributions with mean ranges that

increase with increasing projectile energy and whose values agree with the assump-

tion of complete fusion. The same ' Cf products when produced in the

transfer reaction show angular distributions which peak near the complement of the

grazing angle and show asymmetric range distributions whose mean value decreases
2 l t l 2 5
with increasing projectile energy. The yields of " " C f are much larger in the

transfer reactions compared to the complete fusion reactions. The yields of the

transfer products are described by Hahn et al. with modest success using a modifi­

cation of the semi-empirical Sikkeland systematics of product yields in heavy

17 18
fusion reactions. ' These calculations indicate that the reason for the higher

product yields in the transfer reaction is the relatively cold residual nucleus

produced in this reaction compared to the complete fusion reaction.

Demin et al. used multi-nucleon transfer reactions to produce Ci,

251, 2 5 3 E a > 250, z s * ^ a n d 256 Md f r Q m 2»s cf u 8 i n g 22 N e projectiles. Perhaps

the most significant of the recent "transfer" reaction studies as far as creating

interest in these reactions as useful tools for transuranium nuclide synthesis

20
is the work of Lee et al. Lee et al. measured the yields of heavy actimdes

formed in the interaction of near barrier energy 0, 0, Ne with ^ Cm. In

 - 9
21
follow up to this work Lee e_t a^. measured the excitation functions for the
2
production of isotopes of berkelium through fermium in bombardments of **Cm
1 8
with 0 ions and of isotopes of berkelium through nobelium in bombardments of
2 9 1 8
* C f with 0 ions.
" 22

Schadel e_t a^. measured the distributions of heavy actinide products from
9 2
reactions of ' 0 and Ne with ''Es and found greatly enhanced yields, by many

orders of magnitude, especially for neutron-rich products, of mendelevium and

nobelium isotopes as compared with those produced by the same projectiles with
l,8 2l,9
^ Cm or C f targets. For example the yields of AZ - 2 products - californium

isotopes from '''Cm and mendelevium from Es - were approximately equal, indi­
5<,
cating the tremendous advantage of using a Es target for the production of the

heaviest actinide isotopes.

Apparently, in one reaction mode, at the higher energies, for these transfer

reactions the projectile breaks up elastically in the nuclear field with the

breakup probability having a maximum for the grazing angle (the angle of deviation

fron the original direction for a projectile nucleus making a peripheral collision

with a target nucleus). A fragment of the projectile fuses with the target nucleus,

while the remainder of the projectile carries away a large amount of the available

energy as kinetic energy, thus reducing the excitation energy of the target plus

the absorbed fragment and producing a cold nucleus. The excitation functions

23

appear to be consistent with calculations based on simple energy balance considera­

tions using the masses of the projectile, target nucleus, and products and assuming

the energy of the projectile in excess of the Coulomb barrier is apportioned to

the target nucleus according to the fraction of the projectile mass transferred.

At energies close to the reaction barrier the quasielastic transfer mechanism

apparently prevails.
Extrapolations of the yield curves suggest that higher energy transfer
 - 10

reactions may provide a means of producing new neutron-rich isotopes of known

elements. In this process, at least formally, such tran.i-fer reactions provide

2 2 2 1
a source of exotic projectiles. For example, N e could give rise to F

capture and *0 give rise to ' N capture. This mechanism, with heavier pro­

jectiles such as Ca, might offer another route to superheavy elements.

Somerville e_t aJL have produced a number of interesting isotopes,

that decay via spontaneous fission, by bombarding heavy transplutonium nuclei

with light heavy ions. These include an isotope with a half-life of about 100

milliseconds, produced with the unexpectedly large cross section of a microbarn

l e
by the bombardment of *Ee with 0 ions. Another interesting isotope,
5
presumably °Rf (element 104), produced by the reaction of ' N ions with

Bk nuclei and by other reactions, has been shown by Hulet et al. (when
I 5 2l,9
produced by the reaction of N ions with B k nuclei) to decay with an unusual

symmetric distribution of fission products. This may indicate that the reactions,

and decay of nuclei in this region may be governed by a single fission barrier,

in contrast to the doubly humped fission barrier characteristic of lighter

heavy transplutonium nuclei.

Deep Inelastic Transfer Reactions. For heavy targets and heavy ions with

A < 40, it has been observed that the complete fusion cross section is a very

important part of the reaction cross section. By extrapolation, it was felt

that this situation would continue with projectiles as heavy as krypton. Thus,
2 0 9 8,
the reaction of B i with *Kr was thought to be a possible avenue for pro­

ducing transuranium nuclei. However, it was discovered in the course of this

attempt to make new transuranium nuclei, that the complete fusion cross section

was negligibly small and that a new type of reaction, deep inelastic scattering,

was occurring. This failure of heavy nuclei to fuse is due to the fact that the

Coulomb repulsive forces between the touching nuclei exceed the nuclear attractive
 - 11

forces leading to fusion, resulting in the inability of the nuclei to inter-

27
penetrate inside the fission saddle point. However, it was soon realized that

this new reaction with its characteristic extensive exchange of nuclcons between

projectile and target nuclei during the reaction could lead to significant pro­

duction of trans-target species. The reaction product mass distributions are bi-
28
modal with centroids near the target and proje.-tile masses and with distribution

widths larger for high mass targ ... and projectiles. Also the emission directions

of the products are more complicated than for the other reaction mechanisms. Thus,

deep inelastic transfer reactions involving uranium or heavier targets with heavy

projectiles would be expected to lead to the production of transuranium nuclei

with atomic numbers ranging well above that of the target nuclei.

The most significant use and understanding of deep inelastic transfer

3 8
reactions to produce transuranium nuclei has been in the studies of the U +
2 3 8
U reaction at the UNILAC at GSI. The first realization of the unusual potential

of this reaction for transuranium nuclide synthesis was in the work of Hildenbrand,
29 30
Freiesleben and co-workers. ' who found, from reconstructed primary Z and Q

value distributions, more particle transfer at a given energy loss than in other

systems, i.e., the diffusion process seems to proceed colder in this system. Cold

transfer is, of course, just what is needed to make the fragile transuranium

species. Radiochemical studies by Schadel e^ jsU confirmed thu coldness of the

2 3 8 2 3 8
products from the U + U reaction and its implications.
A somewhat expanded
32
version of these studies has been reported by Gaggeler, e_t aj. The distribution

of target-like fragments from the deep inelastic reaction peaks at Z = 91 rather

33
than Z - 85 (as found in the Xe + U reaction or Z • 79 (as found in the Kr + U

reaction-**). Thus, the "goldfinger" (as this feature was dubbed in Reference 34)

had become the "Protactinium finger". This upward shift «f Z of the peak of the

survivor distribution and its broadening are further indications of the colder
 - 12

diffusion occurring in this system. Reconstruction of the primary target-like

fragment distribution led to an estimation of the production cross section of

2 e 2
2 - 70 fragments in this reaction of 1 0 " cm which, under the assumption of a

binary process, oust also be the estimate of the primary fragment yield of the

superheavy element 114 in this reaction.

The fact that the transuranium element distributions have the same general

shape in the U + U and Xe + U reactions end the fact that the centroids and widths

of the distributions change little with proisctile energy^ can be understood in

terms of the fact that despite changes in the primary distributions with projectile

Z, A and E, only those few nuclei in the low excitation energy, low J angular

momentum tails of the primary distributions will survive fission. The principal

advantage of the U + U reaction is that because of the generally broader primary

product distributions, the number of nuclei in the tails of the distributions

increases enormously.

2 3 8 2 3 8
As a logical followup to the work with the U + U reaction, Gaggeler

et al.32 and Schadel eit a^. have reported the results of attempts to produce
3 8 2<fS
transuranium nuclei in the reaction of 7.4 MeV/u U with Cm. The shapes and
2 3 8
centroids of the isotopic distributions are similar to those observed in the U +
2 3 8 2 3 a 2l 8
U reaction but the magnitudes of the yields are much greater in the U + * Cm
238 2lf8
reaction. For example, the tJ + C m reaction gives 'V'lO'* times more Cf, and
3 2 3 8 2 3 8
10 times more Fm than the U + U reaction. Gaggeler e_t a K ' extrapolate
2
to a 10 fold enhancement in the Md and No yields in the U + "Es reaction and
3
a MO fold enhancement in the Lr yields.

Unfortunately, however, no products beyond Z " 101 were observed even in the
2 3 8 2lf8
U + C m reaction, indicating that the deep inelastic transfer will not provide

a route to new transuranium elements, although it should prov de a route to new

transuranium isotopes.
 - 13

TECHNIQUES FOR IDENTIFICATION OF TRANSURANIUM REACTION PRODUCTS

General. In the study of heavy ion reactions resulting in transuranium

products, it is of paramount importance to be able to isolate and uniquely

identify the products as to their atomic number (Z), mass number (A) and for-
2
nation cross section. Indeed the claim to discovery of a new element must

involve identification of Z while the claim of discovery of a new nuclide must

involve measurement (and/or deduction) of both Z and A. Nitschke has classi­

fied the commonly used techniques of isolating transuranium reaction products by

the half life (t, ) of the products and the minimum detectable cross section. His

classification scheme is shown in Figure 1. Sone of the isolation techniques

shown in Figure 1 such as chemistry, magnetic spectrometers, etc., can also serve

as methods of establishing the Z and/or A of the species involved.

Chemical Methods. For reaction products with the longest half-lives,

chemical separation techniques offer a convenient method of isolating individual

reaction products and establishing their atomic numbers. These tecnniques offer

the greatest sensitivity of all methods because of the large amounts of target

material that can be used.

A typical example of the use of chemical techniques to study heavy ion

38 39
reactions is the effort of Kratz, Herrmann and their co-workers at GSI ' to

study the production of trans-target actinides and possible superheavy elements

3 23
formed in the reaction of U with * U . The chemical problems involved in

these studies are formidable. Because of the large cross sections for deep in­

elastic scattering and the high fissionabilities of the transuranium nuclei, the
7
sought after actinide (Fm, Md) production cross sections are approximately 1 0

less than those of interfering Ra, Ac and Th activities. The separation scheme

used is illustrated in Figure 2 and involved the use of four linked chromato­

graphic columns, three of which involved High Performance Liqi i Chromatography

techniques. A chemical yield of 80-90% with a separation factor of greater than

 - 14
7
10 was achieved. Similar chromatographic techniques were used by Unik et al.

to study actinide production in proton-irridated U targets while ion exchange

41 20

procedures devised by Kratz, Liljenzin and Seaborg and Lee et al. have been

widely used in heavy ion reaction studies at Berkeley.

The Helium Jet. Drums, Tapes and Wheels. For species with half-lives in

the range from 0.1 < t, < 10 Sec, the helium jet is a superior method of isolating

reaction products, as witnessed by its use in the discovery of new elements.

In this method, first developed by Ghiorso e_£ £^., Friedman and Mohr, -* and

McFarlane and Griffoen, *^ reaction products recoiling from the target are

thermalized in helium gas at approximately one atmosphere pressure which leaves

the target chamber via a connection to a low pressure area, creating a "jet or >:

45
stream of helium, (Figure 3). The helium gas stream impinges upon a collection
device such as a tape or wheel or drum which moves the activities to the detectors.

The selectivity of the jet system may be improved by performing a gas phase
46
chemical separation in the jet during transport of the stopped recoils.

Identification of the collected reaction products can be made with a variety

of techniques. Perhaps the most important of these techniques it* the "mother-

daughter" or "double-recoil" method which establishes a genetic link between the

unknown reaction product and known daughter and/or grand-daughter activities. In

this technique (see Figure 3 ) , the recoil heavy atom produced by the alpha-

decay of the collected initial reaction product strikes and imbeds itself in a

"mother crystal". The mother crystal is then moved in front of a "daughter

crystal" which can detect the alpha-decay of the imbedded atom in the mother

crystal. The procedure can be extended to detect additional descendents in t.ie

alpha-decay chain. If the alpha-particle decay r.haracteristic3 of the daughter,

grand-daughter, etc., nuclei are known, then a genetic link is established and

the (Z, A) of the parent are established. This technique was used in the discovery
 - 15

of several elements and isotopes. • ' '

A newer technique of exceptional power to identify the Z of collected

50
reaction products is the X-ray method. In this technique the coincidences

between the alpha-particles emitted by the decay of the collected recoils and

the K X-rays of the daughter nuclei (produced as a result of internal conversion

decay in the daughter) are observed. The energies and relative intensities of

the X-ray lines, ' serve to identify the Z of the daughter, and therefore the

parent nucleus.

For species whose half-lives are in the range 1 «i < t, < 100 ms, '.he

product collection device is placed in close proximity to the irradiated target

and catches the recoils emerging from the target directly. In such systems, the

heavy ion beam after passing through the target will strike the collection sur­

face (drum, tape, etc.). Schematic diagrams of two such collection devices, are
52
nhown in Figures 4 and 5. Unfortunately, such devices offer no selectivity as

to which reaction products are collected, the recoils are usually implanted so

deeply that alpha spectra are those obtained from a very thick source, and it is

difficult to detect the radioactive decay of the reaction products amidst a

high beta-particle background. Therefore these devices are used frequently to

detect new spontaneously fissioning nuclides. Since spontaneous fission cannot,

in general, be used to identify the Z and A of the fissioning system, axperi-

menters frequently resort to arguments based upon nuclear reaction energetics,

systematica and excitation functions to identify the collected products. Such

identifications are generally considered unreliable and make up the bulk of

those identifications classified as E, F and G by the Table of Isotopes

., 53
compilers.

Magnetic Spectrometers, Velocity Filters. The principal problem with the

isolatior devices discussed above (tapes, jets, etc.) is that the reaction pro-
 - 16

duct must be stopped and mechanically transported to radiation detectors before

product identification can occur. This restricts their use to studies of nuclei

whose t, > 1 »«. For detection and identification of species whose t, > 1 ys,

an instrument based upon magnetic and/or electrostatic deflection of target

recoils can be employed. One of the most successful of these devices in recent

years is Che velocity filter SHIP (Separator for Heavy Ion Reaction products)
54 11
located at the UNILAC at GSI. ' A schematic diagram of this separator is

shown in Figure 6. Evaporation residues produced in a nuclear reaction emerge

in the forward direction from the target and pass through a thin carbon foil

which has the effect of equilibrating the ionic charge- distribution of the

residues. The ions then pass through two filter stages consisting of electric

deflections, d pole magnets and a quadrupole triplet for focusing. The solid

angle of acceptance of the separator is 2.7 msr with a separation time for the

reaction products of approximately Z microseconds. Since complete fusion evapora­

tion residues have very different velocities than target-like transfer and deep-

inelastic products, the separator with its ± 5Z velocity acceptance range effect­

ively separates the evaporation residues from other reaction products. Following

separation, the residues pass through a large area time of flight detector and

are stopped in an array of ssven positicn-ssncitive delectus. From their time

of flight and their energy deposit in the position-sensitive detectors, a rough

estimate of their mass may be obtained. The final genetic identification of the

residues is made by recording the correlations between the recoil position in

the detector and subsequent decay signals from alpha or spontaneous fission

decay or even signals from gamma or X-ray detectors placed next to the position

sensitive detector. This device has been used in the discovery of element 107
2I
and element 109 and the identification of the new nuclides * Md, '''Fm and
2 3 1 2
*Cf.
 - 17

Separators like SHIP are quite expensive and represent major instrumentation

projects. A less sophisticated spectrometer which costs considerably less and

provides the capability to measure the formation cross sections, recoil range

distributions and angular distributions of short-lived (t, •* 1 ms> alpha emitters

formed in heavy ion reactions has been described by Dufour et al.

Another type of device used to isolate and identify transuranium nuclei

(t, > 1 us) is the gas-filled mass separator, typified by the separator SASSY
56
(Small Angle Separator System) in use at the Lawrence Berkeley Laboratory.

In this system (Figure 7) the heavy product recoils from a nuclear reaction enter

a helium-filled (1 torr pressure) magnetic spectrometer. The time of flight and

energy of the recoil nuclei are measured, giving a rough determination of the

product mass number. The recoil nuclei which are imbedded in the focal plane

detectors are identified by their a-particle decay and the decay of their daughters.

SASSY has been used to discover a new ssKn isotope produced in the bombardment

of 5oSn nuclei with ssKr projectiles and its efficacy in the transplutonium

region has been demonstrated by its use to observe the production of ^No from
2 0 8
58
the P b C'Ca, 2n) reaction.

Time of Flight (TOF), Decay in Flight (DIF) and Blocking Techniques. To

detect 8p£cic£ whose l i f e t i m e s are 5u&»i.cinLj.<iiiy less uiou 1 miCcusecond, special

techniques must be employed. They include time of flight (TOF) techniques vhich

when combined with a measurement of the product energy will give information about

the product mass number. For suitable mass resolution, the time of flight must

be approximately 10 - 100 nanoseconds. When searching for rare events, some

selection process (like SHIP or SASSY) must be employed to reduce the "background"

levels in the apparatus. The decay in flight technique whose use is described
18 llf
in Reference 59, and the crystal blocking technique, ° ( 1 0 ~ < t, < lo" .«ec)

give very little information about the identity of a reaction product other than

its existence and its approximate lifetime.

 - 18

FUTURE DIRECTIONS

New Technical Development*. Of the chemical isolation and identification

techniques to be used in the future, those capable of being used for short half-

lives are likely to find the most use. The aqueous chemistry and volatility
61
separation techniques that have been used in off-line experiments will need to be

further adapted to on-line operations to make it possible to detect short-lived

products. The use of volatility separation techniques is of particular interest

because some of the superheavy elements have been predicted to be very volatile

(number 112) or quite volatile (number 114) in the elemental (metallic) form.

In addition, chemical isolation and identification techniques will probably use

the more modern physical chemical techniques. An example of these techniques is

the use of lasers to do single atom detection as in the work of Bemis _et al.

to measure the optical isomer shift for the 1 ms spontaneously fissioning isomer
2l,0
Am. The other traditional identification techniques involving genetic

identification via observations of decay chains or direct measurement of product

Z by X-ray or photoelectron detection appear lo be quite applicable to short half-

life species, especially with improvements in detector efficiency. Clearly the

fast isolation techniques such as the magnetic spectrometers or velocity separators

will have special importance particularly if adapted to study transuranium nuclide

production by a variety of different reaction mechanisms. For a number of the

transuranium production methods of the future, new target technologies, similar

65
to those currently used at the ISOLDE facility for p-nucleus reactions, to allow

the use of higher intensity, heavy ion beams, will have to be developed.

Light Heavy Ion Transfer and Deep Inelastic Transfer Reactior-s. As indicated
20,21,22
above, current research in the use of light heavy ion transfer and deep
32,36 . . .
inelastic transfer reactions has progressed far enough to indicate that
2 9
transfer reactions involving heavier targets such as " C f or ""Es could lead to
 - 19

the production of more neutron rich heavy actinides. It should be possible to

produce and identify important new isotopes of transactinide elements. In

addition to the near transactinide elements, the possibility might extend as

far up as the superheavy elements. Hoffman has speculated that in the

2ht
* Ca + Cm
8
reaction one might be able to produce 2 8 8 2
1 1 2 or " l l 3 in a

relatively "cold" manner.

Cold Fusion Reactions. The success in synthesizing elements 107 and 109
8
using cold fusion reactions has revived interest in the use of the * Ca and

Cm reaction to make superheavy elements. Current attempts, still in

1,8 2lf6
progress, to synthesize superheavy nuclei with the Ca + Cn> cold fusion

reaction, are using bombarding energies closer to the interaction barrier.

These collaborative experiments are using off-line chemical, including vola­

tility, procedures and the on-line detection devices SASSY at LBL and SHIP at

GSI. Previous experiments ' that give negative results had been carried out

at approximately 20 HeV above the barrier because theoretical estimates indicated

that beyond a certain critical size of projectile and target an extra energy

above the interaction barrier would be required to fuse the nuclei. The

critical nuclear sizes, above which this "extra push" phenomenon would set in,
2l,8
were not known at the time. If the '"Ca + C m system turned out to be beyond

the critical size, then an extra bombarding energy would be needed for fusion,

but whether this would do more harm than good was an open question. Experimental
73—78
confirmation of the extra push phenomenon is accumulating in recent studies,

and estimates of the critical nuclear reaction sizes are becoming available.
l|8 2l,8
They indicate that the Ca + C m reaction is, indeed, close to the critical

condition, but the qualitative description of the extra push phenomenon and of the

subsequent fission vs. neutron emission competition is not sufficiently precise

 - 20

to enable one, even now, to decide whether an extra bombarding energy would

or would not be advantageous as regards the final probability of making a

superheavy nucleus. It is still necessary to make a careful experimental

study of the relevant cross sections as a function of energy, in a range from

somewhat below to somewhat above the interaction barrier.

Secondary Beams. One interesting idea for using heavy ion reactions to
79
synthesize transuranium nuclei has been put forth by Dufour, Fleury and Bi^bot.

The basic idea is to use a heavy ioo reaction to create an "exotic" secondary

beam with which to do the actual synthesis reaction. The principal difficulty

is that such processes involve the product of the probabilities of two events,

the initial beam generation reaction and the synthesis reaction. However, as

Dufour, Fleury and Bimbot show, there ere some particularly attractive secondary

beam possibilities. For example, with the use of projectile fragmentation

1 2
reactions in the intense 1 0 part/sec 86 MeV/n heavy ion beams at the SC
6
synchrocyclotron at CERN, one might expect to produce C beams with an inten­

sity of approximately 10 part/sec. The use of such neutron-rich secondary beams

in complete fusion reactions might lead to the production of 10-100 atoms/hr

2 6 0 2 6 I
of ' No. Similar studies with proton-rich secondary beams are estimated
2
to produce lO'-lO atoms/hr of ' ' Bk. These examples are only illustra­

tive of the many possibilities.

Exotic TargetB. Because of its large number of neutrons (155) the isotope
2 5 k
E s may be the best route to the synthesis and identification of the super­

heavy elements. This is the case if nuclear species containing 184 neutrons or

very close to 184 neutrons must be produced in order to have a half-life

8
sufficiently long to be detectable. To reach this goal " Ca would have to be

used as the projectile. This combination might produce a nuclear species con­

taining 182 neutrons by a reaction utilizing the one neutron channel (cold

nucleus intermediate) as follows:

 - 21

25 v(,
*Es • Ca - »l 1 1 9 , n

99 20

25<,
The isotope E s is difficult to produce even in microgram quantities,

but it is probably the best available target material. Other possibilities

are more difficult to realize. The isotope Es as target material could

lead to an odd-odd nuclear species with 183 neutrons (even more desirable) but

it would be very difficult to produce more than nanogram quantities reasonably

free of its intensely radioactive precursor ( Es) in the chain of neutron

2 5 5
capture reactions required for its production; the 40-day half-life of Es
2s
is more difficult to deal with than the 275-day half-life of *Es.

Another desirable material is Cm, with 154 neutrons, but this could be

made available only be recovering it from the debris of underground nuclear

explosions, an expensive undertaking. Here the one neutron channel with the

reaction:
25
°Cm + "'Ca - "'116 + n
96 20

would produce a product of smaller atomic number (presumably an advantage) with

181 neutrons.

IMPORTANCE OF TRANSPLUTONIUM RESEARCH

There is much to be learned about nuclear reactions and their products

by continuing and extending the study of the reactions of heavy ions with

tranaplutonium target nuclei. Especially through the use of the heaviest

2l,8 2 U 9 25,| 2 5 0
available target nuclei, such as Cm, C f , and E 8 , and possibly Cm
2 S S
and E s , it will be possible to produce interesting new high Z actinide

and transactinide isotopes. The detemination of their decay properties will

make it possible to determine the role of the 152 neutron shell in this region.

With the competing fission reaction playing a role as a monitor of nuclear

 - 22

temperature it should be possible to reach a better understanding of the

puzzling mechanism of transfer reactions initiated by light heavy ions.

Similarly, the competing fission reaction should provide an additional

dimension in helping to measure the distribution of excitation energy as a

function of the number of nucleons transferred in the deep inelastic transfer

reaction initiated by the heaviest heavy ions, and in studying the degree of

coldness of heavy nuclei produced in fusion reactions. Such information

should also throw light on the behavior of nuclei as a function of angular

momentum.

If it should prove possible to produce and identify superheavy elements,

we will learn much about fission barriers and the nature of closed shells in a

region 01 proton and neutron numbers well beyond where we now have an under­

standing of these quantities. The nuclear decay properties of superheavy

elements are impossible to predict with any degree of accuracy and thus an

experimental knowledge of these properties, and the decay sequences of geneti­

cally related nuclei, would provide information to put our understanding of the

nuclear structure of the very heaviest nuclei on a sounder basis.

The chemical properties of the superheavy elements will be of extra­

ordinary interest because of the importance of relativistic effects in deter-

62
mining their electron configuration. For example, the six 7p electrons are

predicted to be split into two groups, four 7p3/2 and two 7p% electrons, with
2
the splitting between their energies being such that the filled 7p% subshell

will act as a closed shell and additonal 7 p / 3 2 electrons will act as electrons

outside a closed shell. As an example of this effect, element 115 (ekabismuth)

2

is predicted to have its valence electrons in the configuration 7p^ 7pa/2 with

a stable +1 oxidation state, in contrast to the stable +3 oxidation state of

its homologue bismuth. Thus chemists are excited about this possibility of

studying "relativity in a test tube". The chemical properties of the near

transactinide elements which have not been studied so far (nos. 105, 106, etc.)
 - 23

should be compared with those of their homologues (tantalum, tungsten, etc.).

Research concerned with the limits of the periodic table of elements has

been growing more and more demanding as the lifetimes of the isotopes in

question decrease into the millisecond range or less, and the cross sections

for producing them plunge into and below the nanobarn regime. Past progress

in thi^ field has already relied heavily on having available the right targets

and projectiles. There arc many examples where the substitution of one

combination for another can improve the cross sections for making the desired

isotope by orders of magnitude. This situation will become ever more drastic

in the future, when it will be more and more common that a new element or

isotope can only be made in a single, highly specific reaction, involving a

unique combination of target and projectile. In particular, it is clear that

reaching r.he predicted island of superheavy elements will not be easy, and

if this quest is eventually crowned with success, it will most likely involve
21|8 2 S 0 25l, 2 5 S
exotic transplutonium targets such as Cm, Cm, E s or Es. A whole

area of research at the extreme limits of the periodic table may then hinge

on the availability of some such exotic target material: only the laboratory

fortunate enough to have access to such a target will be able to explore this

field of research. If on an expedition you come to a crevasse 20 feet wide

and want to explore the land beyond, you either have a 20+ foot plank

available or you don't reach that land. A 19 foot plank will not do.
 - 24

ACKNOWLEDGEMENTS

I wish to thank Albert Ghiorso, Wladek Swiatecki, Michael Nitschke,

Matthias Schadel, Kenton Moody, Walter Loveland and Jerry Wilhelmy for

reading a draft of this article and suggesCing correcCions and changes Chat

have led to substantial improvement of Chis final version.

This work was supported by the Director, Office of Enezgy Research,

Division of Nuclear Physics of the Office of High Energy and Nuclear Physics

of the U. S. Department of Energy under Contract DE-AC03-76SF0OO98.

 - 25

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 - 31

FIGURE CAPTIONS

Figure 1. Classification of techniques used to isolate transuranium

reaction products by minimum detectable t, and production cro&s

section. See text for a discussion of these techniques. From

(Reference 37).
•i 36

Figure 2. Schematic diagram of chemical procedures used by Schadel et al.

to isolate actinide elements from heavy ion irradiated U targets.

Figure 3. Schematic representation of a "gas-jet" recoil transport assembly.

Thermalized product atoms are transported in the He gas stream and

collected on the periphery of a wheel or other suitable collection

device. Periodically, the wheel is moved to position the spot in

front of the detectors. A "mother-daughter" detector assembly is

illustrated in the lower portion of the figure and is used to

establish a genetic link. From Bemis (Reference 45).

Figure 4 Rotating and scanning drum system for the detection of short­

lived spontaneously fissioning nuclei. From (Reference 52)

Figure 5 Details of a tape system for the collection and detection of

short-lived spontaneously fissioning nuclei. From (Reference 52).

Figure 6 A schematic diagram of the velocity filter SHIP at GSI.

Figure 7 A schematic diagram of SASSY at LBL.

 - 32

a 16 14 12 10 6 4 2 2 4 6
I0" I0" I0" I0" I0" I0~* I0" I0" I0" I I0 I0 I0
T| (sec)
/2
XBL 783-2433

1. Classification of techniques used to isolate transuranium

reaction products by minimum detectable t, and production

cross section. See text for a discussion of theBe techniques.

(From Reference 37).

 U Target

HNO, _i_
Dissolution
1Q2 mHCI/HF
02 mHCI/HF
SI. Cation •F.'CU Complexes D B (
l VPa
2j0mHCI/Cl exchange
o

6mHCI
-TPE,Pu,Ra
6 m HCI 0375m«HIB
-Ac
pH475
Oxalic acid
-Th
-TPE*- Sll Cation •• «-HIB
((Ac)) Ra exchange
SHI Anion •6m HCI
HCI/H^ exchange
*Pu
HN0 3 |0.I8 m HNO3
Figure 2. Schematic diagram of
a) 0.18 m
SIV Extraction
b) 025 chemical procedures used by
chromatography —*»a)b) Washing
Schadel et^ al. to isoiate
HDEHP-HNO: -Am Cm Bk
actinide elements from heavy ion
•Cf Es((Bk)) irradiated U targets.

»Fm
-Md
 HELIUM
TO INLET ABSORBERS
VACUUM
,FOIL 1
INSULATOR^
VVINOOVV
FARADAY
CUP>.
1_ CYCLOTRON
BEAM
Rfrrr,,,.;
RECOILS ^ T A R G E T

NOZZLE

RAPIDLY
MOVABLE
WHEEL-
TO DETECTORS
HIGH - S P E E D
VACUUM
P U M P -t—

1 MOTHER MOTHER Figure 3. Schematic representation of

CRYSTAL CRYSTAl a "gas jet" recoil transport assembly.
"B' A* Thermalized product atoms are transported

*?
in the He gas stream and collected on the
periphery of a wheel or other suitable
collection device. Periodically, the
DAUGHTER ' AIRX

wheel is moved to position the spot

CRYSTAL"D" CYLINDER in front of the detectors. A "mother-
(SPRING daughter" detector assembly is illus­
RETURN) trated in the lower portion of the
DAUGHTER figure and is used to establish a
WHEEL- CRYSTAL "C" genetic link. From Bemis (Ref­
erence 45).
MULTIPLE DETECTOR U N I T
 VACUUM ENCLOSURE
DRUM SYSTEM

WATER COOLING

ROTATIONAL DRIVE MOTOR

WATER COOLING

Figure 4. Rotating and scanning drum system for the detection of short­ XBL 7912-13728

lived spontaneously fissioning nuclei. From (Reference 52).

 - 36

ELECTRICAL^
INSULATION
WATER-COOLED
POST

.025 MM NICKEL TAPE

XBL 799-11395

Figure 5. Details of a tape system for the collection and detection of

short-lived spontaneously fissioning nuclei. From (Reference 52).

 Target Quadrupole c'lectric Dipole Magnets Electric Ouadrupple Detector
Chamber Triplet Field I Field I I Triplet Position

| Entrance Velocity Slit Projectile Beam

Aperture Collector
Carbon Foil
Target

Figure 6. A schematic diagram of the velocity filter SHIP at GSI

 SASSY ( Small Angle Sepa-ator SYstem )

F a s t . . . micro second

High efficiency.. .

£>
E47 oeam line

Target

Detector Array Quadrupole Magnet Bending Magnet

a. Suppression of beam,
a. 2 position sensitive
proportional counters Time of flight
b. Mass separation.

!
b. 10 S crystal array

14 feet from target to focal plane

Recoil energy
Operating in 1 t o r r He
a, S.F

Figure 7. A schematic diagram of SASSY at LBL