The Crystallography,

Metallography and
Composition of Gold
Robert M. Hough1, Charles R. M. Butt1 and Jörg Fischer-Bühner2

1811-5209/09/0005-0297$2.50   DOI: 10.2113/gselements.5.5.297

G
old is an element, a metal and a mineral. In nature, gold most Native gold nearly always occurs as
commonly occurs as an alloy with silver and, more rarely, with an alloy with Ag; natural alloys
with Cu, platinoids, Hg, Pb, Sn, Sb
palladium, mercury and copper, and ranges in size from nanoparticles and Bi are much rarer. Gold and Ag
to nuggets weighing 70 kg. Crystallography, metallography and composition have the same atomic radius and
control the colour of the alloy, how it will deform, how it will behave at high so can form a continuous alloy series;
when the Ag content exceeds 20 wt%,
temperature and how it reacts. These properties offer insights into how gold the alloy is termed electrum. The
deposits have formed and been altered, whether under hydrothermal or variation in the Au/Ag ratio of
Earth-surface conditions. native gold has led to the composition
being described in terms of “fineness”,
Keywords : gold grains, electrum, alloy, annealing, gold nuggets which is represented by the formula
1000 × wt% Au / (wt% Au + wt% Ag).
INTRODUCTION In effect, this describes the gold content of the alloy in parts
Elemental gold is relatively rare (~1 ppb) in the Earth’s per thousand and is a key parameter used to characterize
mantle and continental crust and is a trace constituent gold in hypogene, alluvial and supergene environments.
(~1 ppm) in some meteorites (Palme and O’Neill 2003). As From a few weight percent up to 50–60 wt% Ag, the alloy
a metal, gold has a high melting point, is soft, dense, highly retains its malleability and ductility, but properties such
malleable and ductile, and is an excellent conductor. As a as colour, microstructure, hardness, work-hardening during
mineral, gold is an isometric (face-centred cubic) phase deformation and response to heating are altered.
with a close-packed atomic structure. It takes many crystal
habits, including cubes, octahedra, dodecahedra, triangles Much of the literature on gold deposits ignores the gold
and hexagons. Native gold is found dominantly as small itself, other than giving a chemical analysis. Gold composition
(micrometre- to millimetre-sized), finely disseminated, is discussed in some contexts, but gold’s crystallography
mostly polycrystalline particles and grains and, more and metallography are less commonly considered. This paper
rarely, as single crystals. It also occurs as polycrystalline highlights the significance of these properties to studies of
dendrites, wires, plates, sheets and nuggets (Fig. 1). Many gold ore systems.
of these are exquisite forms and are a result of twinning
controlled by the {111} 60° twin law; for example, wires Au/Ag ratios and primary Gold
(Fig. 1d) are formed by repeated twins. Gold also occurs as Primary (hypogene) gold is gold that has been
a component in other minerals, including tellurides deposited/precipitated from high-temperature hydrothermal
(calaverite, petzite), selenides and sulfides, and as a trace fluids. These either originated deep in the Earth’s crust or
component in, for example, pyrite, arsenian pyrite and were circulating meteoric waters heated at shallower levels.
arsenopyrite. The extensive studies of arsenian pyrite from Ore bodies formed from these systems, or the placers
Carlin-type deposits revealed that incorporation of Au into derived from them, are the most commonly mined deposits.
the pyrite structure is facilitated by As. In this case, Au can Most primary gold is an alloy of Au and Ag, with the Au/
be “invisible” and in solid solution, with a maximum Au/ Ag ratio >1. The gold typically contains 5–20% Ag, but in
As molar ratio of 0.02 (Reich et al. 2005); above this ratio, some deposits, it is essentially pure whereas, in others, the
though, gold can be imaged directly by high-resolution Ag content may exceed 50%. In general, the Au/Ag ratio
transmission electron microscopy as nanoparticles of of primary gold has been little studied. Most reported Au/
metallic Au (Palenik et al. 2004). Such nanoparticles in Ag ratios are <1 (e.g. Boyle 1979) because they derived from
arsenian pyrite have been shown (experimentally) to the ore or from mine bullion, and thus include contributions
become unstable above 370°C; however, if they coarsen from other Ag-bearing minerals. Variable proportions of
during heating, the particles are stable up to 650°C (Reich the Ag are recovered from different ore minerals during
et al. 2006). These observations set an upper limit on the processing; therefore, the Au/Ag ratio differs among ore,
temperature at which the nanoparticles (<4 nm in size) are bullion and primary gold from the same deposit.
likely to exist in such refractory ores. Gold nanoparticles Nevertheless, in the absence of direct analyses of gold,
are clearly an important component of hydrothermal gold these ratios have been used as indicators of evolving fluid
systems, which we are only beginning to understand. chemistry and temperature of deposition, with the more
soluble and volatile Ag becoming enriched in the alloy
higher in the crust and more distally from the centre of
1 CSIRO Exploration and Mining, 26 Dick Perry Avenue
Kensington, Perth, WA 6151, Australia the deposit. An increase in Ag content laterally and towards
Corresponding author: Robert.Hough@csiro.au the surface has been noted in several porphyry deposits,
including Tonopah (Nevada, USA) and Bingham (Utah,
2 Indutherm Erwärmungsanlagen GmbH, Walzbachtal-Wössingen
Germany, and Legor Group Srl, Bressanvido (VI), Italy USA) (Boyle 1979). At Cerro Casale in Chile, variation in

E lements , V ol . 5, pp. 297–302 297 O c tober 2009

A B

C
D E

Figure 1 Hypogene gold: (A) gold with arsenopyrite in quartz, producing deeper yellow colours and a pink to reddish hue
Bayleys Reward, Coolgardie, Western Australia; (B) gold at high Cu content. In contrast, if Ag is present, the drop
nugget, Mount Pleasant, Western Australia; (C) polycrystalline, multiply in the reflectivity curve is shifted towards the high-energy
twinned, fern-shaped gold crystal, Victoria, Australia; (D) wire gold,
Victoria, Australia; (E) two joined single gold crystals, Victoria, Australia end of the visible-light spectrum, giving pale yellow, greenish
yellow, greyish or whitish colours, depending on the Ag
content. Colour variations in the ternary Au–Ag–Cu system
the Ag and Cu concentration in gold was related to are illustrated in Figure 2.
hydrothermal alteration and to specific lithologies (Townley
et al. 2003). Potassic alteration led to higher Ag and lower Constitution, Microstructure and Hardness
Cu contents, and provided the link to show that the gold Deformation of Au, like any metal, takes place by the sliding
associated with this alteration was sourced from a particular of crystal planes over each other through the movement of
granodiorite intrusion. lattice defects, called dislocations. This is particularly easy
The Au/Ag ratio can also indicate temperature. At the for pure gold, which is characterized by a low hardness of
Challenger gold deposit in South Australia, metamorphism 20���������������������������������������������������
–��������������������������������������������������
30 HV (Vickers hardness number) and a high deform-
to 800°C is believed to have melted gold (melting point ability of over 90% in an as-solidified or annealed state.
1064°C) and remobilized it as a result of a lowered eutectic Any distortion of the crystal lattice or any obstacle in the
due to the presence of bismuth (melting point 271°C) and lattice increases the force required to move the dislocations
other components in the gold melt. The low Ag content through the lattice, resulting in an increase in hardness.
(2%) in gold at Challenger could be a result of the Alloying elements and impurities can lead in many different
decoupling of Au and Ag due to their different melting ways to such distortions or obstacles to deformation.
points (Tomkins and Mavrogenes 2002). Silver is completely soluble in liquid and solid Au in all
proportions. The melting temperature decreases gradually
Gold metallography and continuously from 1064 to 962°C, as Ag content
increases from 0 to 100%. This behaviour is directly related
Colour Variation to the close similarity in the atomic radius of Au and Ag,
Gold and copper are the only metals that are not white or so that Ag atoms easily replace Au atoms (and vice versa)
grey in their pure form. A deep drop in the reflectivity in the face-centred cubic crystal lattice. As a consequence,
curve of pure gold occurs within the higher-energy (green the microstructure of Au–Ag alloys is single-phased, and
and blue) part of the visible-light spectrum, resulting in very little hardening of Au is observed with increasing Ag
gold’s yellow colour (Saeger and Rodies 1977). With the content. On the other hand, Cu is ~12% smaller in atomic
addition of Cu, the drop in reflectivity is shifted further radius than Au, resulting in larger distortions when it replaces
towards the low-energy end of the visible-light spectrum,

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Au in the crystal lattice. Hence, even small additions of Cu
lead to significant solid solution hardening of Au. Minor
additions (well below 0.5 wt%) of rare earth, alkali, alkaline
or light metals can harden gold up to ~60 HV in the
as-solidified or annealed state (Corti 1999).

Recovery, Recrystallization and Grain Growth

at Elevated Temperature
During deformation, the microstructure of any metal
becomes strongly distorted and the material is ‘work-hardened’.
If it is subsequently exposed to elevated temperature (say,
between 150 and 500°C), the metal softens again: the
microstructure first recovers by the annihilation of some
lattice defects and the nucleation and growth of new,
undeformed crystals of regular shape. The size of the
resulting crystals depends critically on the degree of
deformation and the temperature; this is shown for pure
gold by the recrystallization diagram in Figure 3. This
process is referred to as annealing.

If deformation takes place at elevated temperature, softening

occurs at the same time, in processes referred to as dynamic
recovery and dynamic recrystallization. As indicated by
Figure 3, (1) low-level deformation followed by annealing
and (2) slow deformation at elevated temperature can both
lead to the growth of large crystals in pure gold. Similar Colour variations in the ternary Au–Ag–Cu system
Figure 2
crystal growth occurs in Au–Ag alloys, such as those found (modified after Grimwade 2000). The colours shown
in natural native gold. However, alloying elements (base are indicative of the actual gold colours. The dashed lines refer to the
gold content of the alloy in carats.
metals) with low solubility in the Au matrix can drastically
reduce grain-boundary mobility, and hence the size of resultant
crystals. This is because the alloying elements tend to
migrate to the boundaries and therefore need to be able to
move with them during recrystallization and grain growth
(Humphreys and Hatherly 2004). Recrystallization and
grain growth can also be inhibited by fine particles formed
by alloy additions, impurities and/or the reaction products
of these materials (e.g. oxides). Depending on particle size
and distribution, such particles can effectively pin and
stabilize grain boundaries, a mechanism referred to as
Zener pinning, and can have a significant influence on
crystal size. The minimum temperature at which annealing
recrystallization occurs increases with the Ag content. For
example, pure gold anneals at about 80°C, whereas an alloy
with 5% Ag anneals at about 250°C. The effect is more
extreme with base metals, which increase the recrystallization
temperature of Au to ~250–400°C even if they are present
at only 0.1–0.5 wt% (Ott 1997).

gold grains
Alloy Composition
Gold grains found in stream sediments and soils have long Figure 3 Recrystallization diagram for pure gold, showing the
been exploited as a resource and used as a guide in exploration dependence of grain size on annealing temperature
and level of deformation. Modified from Degussa et al. (1995)
for primary mineralization. Numerous studies of gold
grains from alluvial and regolith settings worldwide, in a
great variety of geological and geographical environments,
have attempted to link morphology and composition to variable Ag contents, not surprisingly represented Au-rich
process and origin. Morphology has rarely proved diagnostic Cu porphyries. Chapman et al. (2000) found that alluvial
of origin, but is relevant to transport. Compositionally, these gold grains in SW England contained appreciable Pd (3.1%),
deposits are generally of higher fineness than the primary similar to the local primary mineralization. They also
source, due to partial leaching of silver and the precipitation studied mineral inclusions in gold grains to obtain further
of secondary gold. With the advent of micro-analytical insights into source mineralization and the chemical
techniques, the alloy composition of gold is providing nature of the ore-depositing fluid. For example, some grains
information about provenance and genesis. contained selenide and telluride inclusions, rather than
the more common sulphides, which suggested more
Townley et al. (2003) found that the Au, Ag and Cu contents oxidizing conditions were present during one phase of gold
of alluvial gold grains in Chile provided the best link to mineralization. A combination of shape and composition
their source. Silver-rich (5%) grains with low Cu (0.1%) of gold grains was used by Knight et al. (1999) to interpret
were found to come from epithermal systems, and grains distance of transport in stream sediments in the Yukon
even richer in Ag (8%) but with low Cu (0.1%) were from (Canada). They found that the roundness and flatness of
Au-rich porphyries. Grains richer in Cu (up to 0.75%), with grains increased rapidly over the first 5 km of transport

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 from the source. They also measured the development of confirm that, in most cases, Ag depletion is the probable
rims of pure gold on the grains and concluded that these cause. Indeed, the crystallinity of the grains has not been
were due to depletion of Ag from the alloy, not to addition considered in most studies, but it explains the observation
of Au. Together, the extent of depletion and the amount that internal veins and patches of pure gold are controlled
of flattening of the grains provided an indication of whether by crystal structure. The preferential dissolution of the
the grains were proximal or distal to their source and thus more soluble Ag leaves an enriched zone, rarely more than
allowed gold grains to be separated into different populations a few tens of microns thick, on the exposed surface and
related to transport. internally along crystal boundaries. Silver depletion of
alloys has also been described in the jewellery, decorative
Silver Depletion arts and metallography literature (Grimwade 1999). Depletion
The higher fineness of gold recovered from placers and gilding was used by many ancient civilizations to modify
regolith deposits relative to the primary source is manifested the surfaces of artefacts so that they appeared to be made
as external rims and coatings, internal veinlets and void of pure Au. The science of depletion is also exploited in the
walls of pure Au in relict primary Au–Ag grains (Fig. 4a). nanotechnology industry to produce thin films possessing
Whether the veinlets and rims of pure gold are due to novel nanoporous structures with unique properties
secondary precipitation of gold or to depletion of Ag from (Erlebacher et al. 2001; Cobley and Xia 2009 this issue).
the host alloy has long been debated (e.g. Groen et al. 1990).
The intricate structure of some pure gold rims, the lack of Secondary Gold
inclusions, the presence of zones of intermediate Ag Gold precipitated in the surface or weathering environment
concentrations in otherwise homogeneous grains and the is referred to as secondary or supergene gold. Most
recent observation (Hough et al. 2007) that, internally at secondary gold is nearly pure (i.e. of high fineness),
least, these zones and veinlets follow crystal boundaries, containing <1% Ag (Freyssinet et al. 2005). It can thus
generally be differentiated from primary Au–Ag alloy,
although rare secondary electrum is reported from some
A environments (Webster and Mann 1984; Clough and Craw
1989). Secondary gold has been found in soil, deep regolith,
stream sediments and placers, from the Arctic to the humid
tropics; it commonly forms delicate structures – convincing
evidence for growth in situ. Gold can be mobilized as complexes
with several organic and inorganic ligands (Freyssinet et
al. 2005). Secondary gold probably precipitated from
organic complexes occurs widely in tropical swamps, soils
and lateritic regoliths (e.g. Ashanti, Ghana; Bowell 1992).
However, where similar lateritic regoliths are preserved in
now semi-arid regions with acid, saline groundwater, such
as in Western Australia, the formation of gold halide
complexes has led to strong leaching, followed by the
concentration of secondary gold as mineable deposits over
sub-economic primary mineralization. In these deposits,
some secondary gold is coarser than most of the underlying
primary gold. The secondary gold has precipitated as
euhedral crystals with a variety of habits: aggregates with
very delicate fern-like and dendritic structures, and wires
and plates. Despite these ‘coarse’ forms, much secondary
gold is very fine grained and essentially ‘invisible’, probably
B
forming sub-micron-sized particles in Fe–Mn oxides, clays,
carbonates and sulfates (Freyssinet et al. 2005). Even in such
cases, trace analysis by laser ablation ICP–MS shows the
secondary Au to be particulate: in transects across samples
of Au-bearing laterites and calcretes, the Au profile is spiky
rather than a plateau (Lintern et al. 2009). Once reduced
from solution or colloid, gold is particulate at all scales, to
nanometres or less.

Much secondary gold has precipitated as single crystals

with hexagonal or triangular habit. These forms are abundant
in saline environments (Lawrance and Griffin 1994) and
are reminiscent of those resulting from the reduction or
evaporation of Au colloids in the laboratory and imaged
by transmission electron microscopy (Sun and Xia 2002;
Noble et al. 2009). In such studies, various organic compounds
and bacteria have been used to reduce Au chloride solutions
to form colloids, from which nanoplates and nanoparticles
of pure Au can ultimately be deposited. Identical colloidal
Figure 4 Back-scattered electron images. (A) Silver depletion
(labelled) in the interior of an etched Au–Ag nugget gold crystals have been observed occurring naturally in
from Queensland, Australia. The depletion proceeds along crystal weathering gold deposits in Western Australia, where
boundaries and also affects specific crystals. Inset: same polished highly saline, Au-rich groundwaters are precipitating
surface prior to etching; Ag depletion shows as bright features. visible Au plates (100–300 µm) (Fig. 4b) at the water table
Specimen (repolished and etched) from the Liversidge Collection, courtesy
of the N atural H istory M useum, London (B) Single secondary Au
(Hough et al. 2008). These plates host a nanoparticulate
crystals from the Golden Virgin deposit, Western Australia (the population of hexagonal and triangular gold crystals as
differing white and grey shades are due to thickness variation). small as 50 nm. The Au crystals grow in the colloid by a

E lements 300 O c tober 2009

twinning-controlled mechanism, forming thin triangular
A
and hexagonal plates in a single evaporative event. These
attain their maximum thickness early during growth
(within 24 hours) and then grow laterally.

The nugget controversy

Gold nuggets have long captured the popular imagination.
To the public and prospectors, they represent a romantic
and fortuitous route to instant wealth; to geologists, they
are a curiosity of imprecisely known origin. Defined as
masses weighing >1 g or measuring >4 mm, nuggets were
commonly discovered during the early gold rushes in
North America and Australia. By far the majority came
from alluvial deposits and regions with a deeply weathered,
residual regolith. The Victorian goldfield of southeastern
Australia was the most prolific source, producing both the
greatest numbers and the largest. By 1910, at least 1200
nuggets weighing, each, more than 20 troy ounces (622 g)
had been documented; many exceeded 1000 oz (31.1 kg),
and the two largest, the Welcome and the Welcome Stranger,
were 2218 oz (~69 kg) and 2315 oz (72 kg), respectively.
Large nuggets are still being found today (Fig. 5).

Figure 5 This 8 kg gold nugget (Kingower, Victoria, Australia)

was found in the near surface with a metal detector in 1995.

The origin of nuggets has been debated for over 160 years,
but very little scientific study has been carried out. Many
prospectors and geologists consider most nuggets to be
secondary, formed in alluvial or weathering environments.
Their relative abundance in these environments compared
to their rarity in lode deposits, the rounded or mamillary
form of some nuggets and the overgrowths on others, as
well as observations of delicate structures and small pristine
crystals in recent sediments support a supergene origin.
The early debate was summarized by Liversidge (1893) who,
although demonstrating that gold could be dissolved in
groundwater and reprecipitate under surface conditions,
nevertheless concluded on geological grounds that nuggets
in alluvium and weathered rock are of primary origin. He
also showed that nuggets are internally polycrystalline
(Liversidge 1897). Unfortunately, Liversidge’s conclusions
and, in particular, his petrographic observations and
techniques were forgotten. Wilson (1984) incorrectly
concluded that nuggets from Western Australia had accreted Figure 6 A section of a nugget from Bayleys Reward, Coolgardie,
Western Australia, imaged by optical microscopy: (A)
around secondary Fe oxides and clays, but Wilson did not polished, (B) polished and etched. Etching reveals a polycrystalline
etch his specimens and saw only featureless, shiny surfaces, structure, with twinning diagnostic of annealing. The ferruginous
not the crystals, the twins and the relationship of secondary material is not enclosed but entered through numerous interconnecting
minerals to crystal boundaries and the exterior (Fig. 6). voids that are open to the exterior. Specimen courtesy of Queensland
Museum, Brisbane

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The ‘inclusions’ actually occupy voids dissolved by weathering CONCLUSIONS
solutions that had permeated along these boundaries, over
As gold is both a mineral and a metal, any study needs to
a distance of 30 mm in some large nuggets. The dissolved
take into account both its crystallography and its composi-
gold was leached, some precipitating elsewhere as secondary
tion because these play a key role in understanding its
crystals.
physical properties and behaviour (i.e. its metallography).
Recently, Hough et al. (2007) studied nuggets from a wide Metallography provides insights into the features displayed
range of geological and secondary environments, mainly by natural gold, such as grain size, annealing fabrics and
in Australia, and subsequently re-examined those studied colours of alloys. These, in turn, may assist in exploration,
by Liversidge and Wilson. Nearly all are Au–Ag alloys similar by identifying the provenance of detrital particles, and in
in compositions to primary gold, with Ag depletion on paragenesis, by providing constraints relating to the
crystal boundaries open to the exterior. The nuggets have even- thermal and tectonic history of deposits. We are only now
textured, polycrystalline fabrics, with many crystals exhib- beginning to realize the extent of the distribution of nano-
iting coherent and incoherent twinning (Fig. 6). Petrovskaya particulate gold in ore systems. Potentially, nanoparticulate
(1973) provides numerous examples of hypogene and allu- gold may play an important role in the transport and depo-
vial gold from Russia with similar crystallographic features. sition of gold in both hydrothermal and supergene envi-
These textures and fabrics are the same as those observed ronments and lead to improved understanding of the
in metallographic studies, where they are considered char- genesis of deposits in these environments.
acteristic of thermal annealing of Au–Ag alloys at >250°C.
These similarities conclusively demonstrate a hypogene ACKNOWLEDGMENTS
origin for the nuggets. The relative abundance of nuggets We are indebted to our late colleague Ernie Nickel for many
in surficial environments is due to physical concentration insightful discussions over the last few years. Ernie passed
by chemical wasting and fluvial transport, not by chemical away whilst this paper was being completed. Financial
growth. Nuggets are weathering, not forming, in the super- support was provided by the CSIRO Minerals Down Under
gene environment. National Research Flagship.

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