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The Agios Georgios argentiferous galena


deposit on Antiparos Island, Cyclades, Hellas
and its relationship to the...

Article in Neues Jahrbuch für Mineralogie - Abhandlungen · July 2015


DOI: 10.1127/njma/2015/0283

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E N. Jb. Miner. Abh. (J. Min. Geochem.)
Published online April2014
Stuttgart, December 2015
Geochem.)  PrePub Article

The Agios Georgios argentiferous galena deposit on


Antiparos Island, Cyclades, Hellas and its relationship to the
Paros leucogranite

Elias Kevrekidis, Karen St. Seymour, Stylianos Tombros, Degao Zhai, Jiajun Liu,
Dimitrios Zouzias

With 10 figures and 14 tables

Abstract. The Agios Georgios argentiferous galena deposit on Antiparos island lies ~12 km from the Miocene Paros pluton and is
hosted by mineralized quartz veins in marbles of the Cycladic Blueschist Unit. Argentiferous galena and clear quartz were depos-
ited in the epithermal stage in veins armoured by higher temperature milky quartz. The Paros pluton is a mesozonal volatile-rich
tourmaline and Li-bearing muscovite leucogranite emplaced at ca. 700 °C and 4 – 5 kbars. Fluid inclusion microthermometry of
vein quartz yielded ore fluid temperatures from 130° to 400 °C, salinities from 4.8 to 15.7 NaCl wt. percent equivalent and pres-
sures of 100 to 135 bars. CO2-effervescence of the ore fluid at the high end of the temperature range is suggested by Raman data
along with CO2 clathrate formation. Closure and boiling and reopening of the mineralized quartz veins occurred between 240° to
290 °C. Raman spectroscopy of fluid inclusions showed significant contents of Cu2+ and SO42 – indicative of the mineralization and
of Li+, and B3+indicative of magmatic fluid contribution. Raman ratios, i.e., logO2/H2O indicate mixing with meteoric water. Stable
isotope analyses of vein quartz yielded δ18OH2O and δDH2O values of the hydrothermal fluid from 1.2 to 11.6 and –73.2 to – 52.4
per mil, respectively, and δ30Si from – 0.6 to 0.0 per mil. All are consistent with a dominant magmatic origin of ore fluids. The
physicochemical conditions of the ore deposition were pH = 3.6 – 5.5, logfS2 = – 9.7 to –7.3 and logfO2 = – 31.3 to – 34 for 330° and
210 °C and pressures 135 bars. The volatile–rich nature of the Paros pluton, the presence of granitophile elements such as Li+ and
B3+ in fluid inclusions in the vein quartz, the high salinities of the fluid inclusions, the initial high T (> 400 °C) of the mineralizing
event and the magmatic signature of stable isotopes in mineralized vein quartz suggest that mineralizing fluids were derived from
the leucogranite.

Key words: Paros leucogranite, Antiparos epithermal mineralization, fluid inclusions, Raman, stable isotopes

Introduction continent (Mastrakas 2007, Salemink 1985, Salemink &


Schuiling 1987, ST. Seymour et al. 2009a, 2009b, Tom-
Plutons of an overall granitoid composition were em- bros et al. 2008). The leucogranite of Paros is a typical
placed during the Miocene in the back-arc region of the example of the S-type leuocogranites in the Cyclades.
Quaternary Aegean Volcanic Arc in the Cycladic micro- Mining activity in Paros was mostly associated with
continent (Altherr et al. 1982, Altherr & Siebel 2002, the extraction of superb quality marble since antiquity,
Bolhar et al. 2010, Keay et al. 2001) These plutons dis- from which renowned artifacts such as the Hermes of
play I and S-type affinities and in a number of cases I-type Praxiteles were sculpted. However, in Antiparos, which
granodiorites and S-type leucogranites co-exist and each formed probably a single island with Paros in the geo-
is associated with a distinctive mineralization (Mastra- logical past, sulfide mineralization and particularly ar-
kas 2007, Salemink 1985, Salemink & Schuiling 1987, gentiferous galena was mined from metalliferous quartz
Skarpelis 2007, ST. Seymour et al. 2009a, 2009b, Tombros veins at Agios Georgios, which occur in marbles and mica
2008, Tombros et al. 2008). The S-type leucogranites are schists of the Cycladic Blueschist Unit (CBU).
H2O- and volatile (B, F)-rich, and commonly associated In the present study we investigated the origin of the
with hydrothermal mineralization in the Cycladic micro- mineralizing fluids in the Agios Georgios deposit and the
© 2015 E. Schweizerbart’sche Verlagsbuchhandlung, Stuttgart, Germany www.schweizerbart.de
DOI: 10.1127/njma/2015/0283 0077-7757/2015/0283 $ 0.00
 2 E. Kevrekidis et al.

possible genetic link with the Paros leucogranite which is of a succession of Alpine nappes, overlying a Hercynian
located 12 km away. To achieve this objective we deter- meta-igneous basement which consists of gneisses and
mined the petrochemistry and mineral chemistry of the schists (Jolivet et al. 2010, Van Hinsbergen & Schmid
leucogranite, and estimated the physicochemical condi- 2012). These lithologies are intruded by Miocene plutons
tions of ore formation with the aid of fluid inclusion mi- (Altherr & Siebel 2002, Bolhar et al. 2010). On Paros,
crothermometry and Raman analyses, and stable isotope zircon U-Pb dating of ortho- and para-gneisses yield typi-
analyses of vein quartz. cal Hercynian igneous crystallization ages that range from
300 to 315 Ma (Engel & Reischmann 1998, Bargnesi et
al. 2013).
Regional geology The basement is overlain by the Cycladic Blueschist
Unit (CBU). The CBU represents lithologies of a Meso-
The islands of Antiparos and Paros are part of the Cy- zoic continental margin which comprises a Pre-Alpidic
clades Blueschist Belt located in the central Aegean basement, i.e., the Basal Unit (Avigad & Garfunkel 1991)
(Blake et al. 1981). The Cyclades Blueschist Belt consists overlain by a volcanosedimentary sequence (Bröcker &

Fig. 1. Geological map of Paros and Antiparos (Adapted from Kevrekidis 2013).
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 3

Fig. 2. Structural map of the Agios Georgios area (box in the inset) showing the anticline which concentrated the mineralizing fluids.
Schmidt nets of foliation and joints used by mineralizing fluids. A1 to A11 mark metalliferous veins.

Franz 2005). The CBU is locally overthrusted by the Up- part of Paros. Kinematic markers at the fault plane indi-
per Unit which is composed of ophiolites (Katzir et al. cate a top-to-the-NE sense of movement (Gautier & Brun
1996, Jolivet et al. 2010). 1994). The hanging-wall comprises part of the Upper Unit
The CBU has undergone at least two metamorphic composed of Pliocene sedimentary rocks and an ophiolite
events. The first was is dated between ~ 53 to ≤ 40 Ma, slice covered by Cretaceous limestones (Sánchez-Gómez
by 40Ar/39Ar radiometric data from white mica, with con- et al. 2002).
ditions equivalent to eclogite and epidote-blueschist fa- Antiparos and Paros are separated by a narrow graben
cies (Wijbrans & McDougall 1986 and 1988, Ring et and it is likely that these two are part of a former single
al. 2001). Metamorphic temperatures ranged from 450° island. The lithology of the two islands is almost identical
to 550 °C and the pressures were equal to 12 – 20 kbars (Figs. 1 and 2). Antiparos is dominated by CBU schists
(Ring et al. 2001). The second metamorphic event has and marbles, but, it has less marbles than Paros and is
been dated between ≥ 25 and ~12 Ma, by 40Ar/39Ar radi- completely devoid of basement gneiss (Figs. 1 and 2).
ometric data from muscovite (Keay et al. 2001, Bolhar On Paros an S-type leucogranite and pegmatitic dykes
et al. 2010). The temperatures during this event peaked intrude the entire sequence (Fig. 1, e.g., Thapsana site).
at 670° to 700 °C and pressures ranged from 4 to 7 kbars Antiparos displays no exposed granitic intrusions with the
(Wijbrans & McDougall 1986, 1988, Bröcker & Franz exception of a few pegmatitic dykes, of similar mineral-
2005). Greenschist-facies retrogression of the CBU rocks ogy to those on Paros, encountered during fieldwork in
partially overprinted and locally destroyed the high-pres- this study. Early Pliocene rhyolites occupy the southern
sure assemblages of the first metamorphic event (Mat- part of the island (Innocenti et al. 1982) (Fig. 2).
thews & Schliestedt 1984, Schliestedt & Matthews
1987). Miocene granitic intrusions were emplaced dur-
ing and immediately after the second metamorphic event The Agios Georgios vein system
(Altherr et al. 1982, Altherr & Siebel 2002). In Paros,
the intrusive event was dated at 15.5 ± 0.3 Ma based on The Agios Georgios vein system is hosted in biotite-mus-
238 206
U/ Pb radiometric data (Bargnesi et al. 2013). covite schists and marbles of the CBU (Tombros 2008,
Kevrekidis 2013). The main tectonic element in the area
of Agios Georgios is an open anticline (Fig. 2) whose axis
Geology of Antiparos and Paros plunges at shallow to moderate angles towards the SSE
(Kevrekidis 2013, Evans & Fischer 2012). Foliation dips
On Paros, the CBU consists of gneisses, amphibolites, towards WSW to SSE at shallow to moderate angles and
schists and marbles and the Upper Unit is composed of to ENE at moderate to steep angles. Formation of the anti-
meta-dolerites, marbles, calc-schists and phyllites (Papan- cline caused a decrease of lithostatic pressure in the axial
ikolaou 1980 and 2009, Gautier & Brun 1994, Sánchez- hinge zone, which may have drawn hydrothermal fluids
Gómez et al. 2002). A low angle ductile to brittle normal into the area of Agios Georgios (Evans & Fischer 2012,
fault is exposed at the top of the CBU in the northeastern Kevrekidis 2013). The tectonic domain in the Agios Geor-
 4 E. Kevrekidis et al.

gios area consists of a conjugate system of NE-trending Crustification is present in quartz veins which are
sinistral and NW-trending dextral strike-slip faults. There more than 10 cm wide. Two zones of crustification, re-
are two main systems of joints. The first trends NNW and ferred to here as Type A and B bands, have been dis-
dips steeply towards the ENE, while the second trends tinguished based on mineralogy, grain size and texture.
WNW and dips SSW at moderate angles. The generalized sequence of vein crustification (Table
The Agios Georgios vein system consists of eleven 10), from the vein margins to the center is: (Type A): fine-
steeply dipping quartz veins (Fig. 2). Both marbles and to medium-grained drusy milky quartz (> 70 vol.%) with
schists are cut by two generations of syntaxial veins, angular to subrounded fragments of marble and schist.
an older NE-trending set filled with milky quartz and a This band contains also epidote, ankerite, calcite, chlo-
younger set of clear quartz veins trending NW (Fig. 2). rite, sericite and rare orthoclase, albite, as vein filling,
These veins developed parallel to the planes of folia- and (Type B): medium- to coarse-grained clear quartz,
tion and joints, and also along the lithological contacts smithsonite (≤ 20 vol.%), barite (≥ 30 vol.%) and fluo-
between marble and schist, forming extensive stock- rite, which display well-developed open-space filling and
works. Milky quartz veins range up to 80 cm in width, dogtooth textures.
and contain sphalerite, pyrite and chalcopyrite (10 vol.%). Alteration haloes occur around quartz veins, with
The clear quartz veins form tension gashes up to 50 cm widths ≥ 30 cm, developed as discontinuous borders and
in width within the center of the milky quartz veins, and linear selvages in marbles and schists of the CBU. The
they contain galena (≤ 10 vol.% with Ag 800 – 2000g/t) as alteration assemblages define two successive zones: an
the main ore mineral (Tombros 2008, Kevrekidis 2013). inner milky quartz-epidote zone with ankerite, dolomite,

Table 1. Chemical analyses of Paros leucogranites and a mafic inclusion (2). Major elements in wt.%, trace elements in ppm. Below detec-
tion limit: (b.d.). Not determined: (n.d.).
wt.%   1    2   3   4   5   6   7   8   9  10  11  12
SiO2  70.64   55.02  67.67  75.4  74.04  72.35  67.91  70.7  71.2  68.5  70.44  78.04
TiO2   0.31    0.53   0.75   0.03   0.06   0.28   0.57   0.48   0.33   0.6   0.31   0.07
Al2O3  14.86   19.88  14.38  14.93  14.87  15.42  16.7  15.5  15.6  16.2  15.83  12.87
Fe2O3   2.17    4.82   3.91   0.53   0.63   1.72   3.02   2.62   2.25   3.37   1.94   0.71
MnO   0.04    0.05   0.05   0.08   0.01   0.03   0.03   0.02   0.03   0.33   0.04   0.02
MgO   0.56    0.78   1.23   0.08   0.16   0.37   0.86   0.79   0.7   1.07   0.37   0.08
CaO   1.99    3.5   4.56   1.21   1.1   1.94   2.74   2.6   2.08   2.94   2.27   0.86
Na2O   3.48    4.91   2.97   4.24   3.26   3.6   3.51   3.07   4.25   3.24   4.47   3.24
K2O   4.36    6.34   2.89   3.87   5.24   4.19   3.84   4.21   2.56   3.43   4.15   4.36
P2O5   0.11    0.03   0.19   0.04   0.05   0.09   0.17   0.14   0.11   0.18   0.09   0.03
LOI   0.64    4.16   0.89   0.3   0.28   0.39   0.54   0.48   0.65   0.52   0.51   0.44
Total  99.15   99.99  99.49 100.31  99.41  99.98  99.34 100.16  99.82  99.58  99.9 100.27
Sc   3 b.d.   6   6   5   8   9   6   3   6   6  11
V   8   51  33  10  10  17  24  21  20  20  13   8
Cr  20 n.d. n.d.   8 b.d.  24   2 b.d. b.d. b.d.   4   1
Co   2    4   6 b.d. b.d.   3   6  33  43  42   2 b.d.
Ni  20 n.d. n.d. b.d. b.d.   0   1 b.d. b.d.   1   0   0
Cu  80   20  10 b.d. b.d. b.d.   1 b.d. b.d.   4 b.d. b.d.
Zn  60   60  70  17  21  34  50  49  60  67  43  39
Ga  23 n.d. n.d.  20  20  22  23  19  23  24  22  15
Rb 185   84 140 214 207 214 159 170 127 151 190 164
Sr 244  354 413  68 159 242 383 367 254 412 253  43
Y  28    5  13  28  36  11  15  15  18  16   9  55
Zr 191 1676 422  57  47 169 318 315 203 346 179  49
Nb   9   64  19   8  24   9   9  10  13  11  10   8
Ba 717 1376 445  87 438 552 976 992 422 875 552 110
Th  17.2    2.5  18.3   8  13  14  19  20  13  17  11   9
Pb  48    5  29 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 5

Table 2. Rare Earth analyses of Paros leucogranites and a mafic inclusion (Numbers of specimens as in Table 1).
ppm  1  2   3  4  5  6  7  8  9 10 11 12
La 38  9.7  65 10 10 17 35 34 21 31 21 13
Ce 71 17 126 18 10 32 74 62 42 59 37 33
Pr  7.54 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Nd 26 64  50  8  2  9 24 23 18 19 12 15
Sm  4.7  1.2   9.4 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Eu  0.83  0.43   1.25 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Gd  3.3 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Tb  0.5  0.2   1.1 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Dy  2.6  0.9   5.9 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Ho  0.5 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Er  1.4 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Tm  0.2 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Yb  1.3  0.7   2.7 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
Lu  0.8  0.11   0.39 n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d. n.d.
LaN/LuN  0.54  0.99   1.89  –  –  –  –  –  –  –  –  –
LaN/YbN  2.16  1.02   1.78  –  –  –  –  –  –  –  –  –
Y/Ho 28  –    –  –  –  –  –  –  –  –  –  –

(n.d.: Not determined)

Fig. 3. Compositional features of the Paros leucogranite whole-rock samples. a – Most samples of the Paros leucogranites plot in the
peraluminous field on the SiO2-A/CNK diagram (A/CNK equals molar Al2O3/(CaO+Na2O+K2O), metaluminous and peraluminous fields
from Maniar & Piccoli 1989); b –In the Y vs. Nb discrimination diagram samples from the Paros leucogranite plot in the Volcanic Arc and
Syncollisional fields (VAG: Volcanic Arc Granite, syn-GOLG: Syn-Collisional Granite, ORG: Orogenic Granite and WPG: Within Plate
Granite, fields from Pearce et al. 1984); c – Paros leucogranites display LREE-enrichment. Plagioclase fractionation is depicted by the
distinct negative Eu anomaly on these profiles. Normalization values from Nakamura (1977).
 6 E. Kevrekidis et al.

Fig. 4. The composition of minerals in the Paros leucogranite. a – Amphiboles evolve from these of magnesio-hornblendes towards horn-
blende-actinolite (Act: Actinolite, Tsch: Tschemarite, Hbl: Hornblende, Tsi: Tetrahedral silicon, fields from Leake 1978); b – Biotite plots
near the divide between biotite and phlogopite (fields from Guidotti 1984). c – Feldspar compositions from the leucogranite are mostly
andesine-oligoclase plagioclases, with oligoclase rims. K-feldspars plot near the orthoclase apex.

calcite, rhodochrosite, siderite, pyrite, sericite, chlorite Superprobe 8600-L instrument equipped with wavelength
and albite; and an outer clear quartz-barite-fluorite zone dispersive spectrometers (WDS) with EDS and SEM facil-
with galena, rare kaolinite and Mn- and Fe-oxides and hy- ities. Electron microprobe work on petrographic polished
droxides. thin sections was carried-out at an acceleration voltage of
15 kV, a beam current of 20 nA and a beam diameter of 5
μm at 20s counting times. Online ZAF corrections were
Analytical methods done utilizing the CAMECA software. Shorter counting
times (10s) were used to avoid devolatilization of the al-
A total of twelve samples of Paros leucogranite have been kalies from the feldspars. Natural and synthetic feldspars,
analyzed for major and trace elements (Table 1) including diopside, rutile, chromite, hematite, spessartine, fluorite
REE (Table 2). Analyses were carried out by ACTLABS and vanadinite were used as standards. For the feldspars,
laboratory at Ancaster, Ontario, Canada, by ICP and ICP/ the detection limits are: 0.03 wt.% for Si, 0.05 wt.% for
MS methods using code 4Litho research. Detection limits Ti, 0.02 wt.% for Al, 0.04 wt.% for Fe, 0.02 wt.% for Mg,
are 0.001 wt.% for TiO2 and MnO and 0.01 wt.% for the 0.03 wt.% for Ca, 0.07 wt.% for Na, 0.03 wt.% for K and
rest of major elements; 1 ppm or better for Sc, Be, Co, Ga, 0.03 wt.% for Ba. For biotite and amphibole, the detection
Nb, Sb, Cs, Hf, Ta, Tl, Bi, Sn, Th, U and W; 2 ppm for Sr, limits are: 0.03 wt % for Si, 0.06 wt.% for Ti, 0.06 wt.%
Y and Rb; 3 ppm for Ba and 4 ppm for Zr; 5 ppm for V for Cr, 0.03 wt.% for Al, 0.05 wt.% for Fe, 0.05 wt.% for
and Pb; 10 ppm for Cu, 20 ppm for Cr and 30 ppm for Zn. Mn, 0.02 wt.% for Mg, 0.04 wt.% for Ca, 0.03 wt.% for
Detection limits are 0.05 ppm for Pr, Eu, Tm and Lu and Na, 0.02 wt.% for K, 0.09 wt.% for F and 0.01 wt.% for
0.1 ppm for the rest of the REE. Cl.
Mineral chemistry was determined by electron mi- Operating conditions for sulfide minerals were an
croprobe at McGill University, Montréal, using a JEOL accelerating voltage of 20 kV and a beam current of
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 7

Table 3. Microprobe single point chemical analyses of amphibole from the leucogranite of Paros (from sample 1 of Table 1).
wt.%  1  2  3  4  5  6  7  8  9 10
SiO2 47.07 46.53 45.69 47.13 48.23 48.80 48.82 49.79 44.87 45.58
TiO2  0.90  0.98  1.14  0.94  0.81  0.73  0.72  0.64  1.07  1.15
Al2O3  7.33  6.90  7.77  6.60  5.88  5.46  5.29  4.69  8.44  8.01
FeO 14.78 14.73 14.96 14.37 13.71 13.63 13.57 13.27 15.39 15.17
Cr2O3  0.08  0.05  0.06  0.10  0.02  0.08  0  0.01  0.29  0.09
MnO  0.76  0.96  0.84  0.90  0.96  0.93  0.99  0.99  0.80  0.83
MgO 13.33 13.30 12.70 13.56 14.10 14.40 14.44 14.89 12.34 12.54
CaO 11.61 11.47 11.53 11.55 11.52 11.59 11.65 11.57 11.63 11.51
Na2O  1.48  1.45  1.54  1.34  1.25  1.16  1.13  1.05  1.35  1.46
K2O  0.78  0.77  0.89  0.74  0.61  0.55  0.55  0.47  0.94  0.90
Total 98.13 97.13 97.12 97.23 97.09 97.33 97.16 97.37 97.12 97.24
Number of ions on the basis of 23 oxygen atoms
Si  6.95  6.95  6.85  7.01  7.14  7.20  7.21  7.31  6.74  6.83
Al  1.05  1.05  1.15  0.99  0.86  0.81  0.79  0.69  1.26  1.17
Fe3+  0  0  0  0  0  0  0  0  0  0
Ti  0  0  0  0  0  0  0  0  0  0
Sum T  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00
Al  0.22  0.17  0.22  0.17  0.17  0.14  0.13  0.12  0.24  0.24
Cr  0.01  0.01  0.01  0.01  0  0.01  0  0  0.03  0.01
Fe3+  0  0  0  0  0  0  0  0  0  0
Ti  0.10  0.11  0.13  0.11  0.09  0.08  0.08  0.07  0.12  0.13
Mg  2.93  2.96  2.84  3.01  3.11  3.17  3.18  3.26  2.77  2.80
Fe2+  1.73  1.76  1.81  1.71  1.63  1.60  1.61  1.55  1.84  1.82
Mn  0  0  0  0  0  0  0  0  0  0
Ca  0  0  0  0  0  0  0  0  0  0
Sum C  5.00  5.00  5.00  5.00  5.00  5.00  5.00  5.00  5.00  5.00
Mg  0  0  0  0  0  0  0  0  0  0
Fe2+  0.09  0.09  0.07  0.08  0.07  0.08  0.07  0.08  0.10  0.08
Mn  0.10  0.12  0.11  0.11  0.12  0.12  0.12  0.12  0.10  0.11
Ca  1.81  1.79  1.83  1.81  1.81  1.81  1.81  1.80  1.80  1.82
Na  0  0  0  0  0  0  0  0  0  0
Sum B  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00
Ca  0.02  0.04  0.02  0.03  0.02  0.03  0.03  0.02  0.08  0.03
Na  0.42  0.42  0.45  0.39  0.36  0.33  0.32  0.30  0.39  0.42
K  0.15  0.15  0.17  0.14  0.12  0.10  0.10  0.09  0.18  0.17
Sum A  0.59  0.61  0.64  0.56  0.49  0.46  0.46  0.41  0.66  0.63

30 nA. Twenty seconds counting time was used for all ele- sample was also analyzed for δ34S in the latter lab. Oxy-
ments, except Ag (100s) and As (50s). Pyrite, sphalerite, gen was released from milky and clear quartz using the
galena, chalcopyrite, Ag-metal, Au-metal, diopside, spes- BrF5 extraction technique of Clayton & Mayeda (1963)
sartine, stibnite and synthetic CoNiAs were used as stand- and Friedman & O’neil (1977). Hydrogen was released by
ards. Detection limits in wt.% were: 0.042 for Ag, 0.054 thermal crushing from fluid inclusions and structurally
for Zn, 0.048 for Fe, 0.061 for Sb, 0.022 for S, 0.066 for bound waters to minimize fractionation effects as their
As, 0.072 for Cu, 0.037 for Au, 0.046 for Co, 0.207 for Pb, water contents were ≥ 0.2 wt.% (≥ 1000 μmol H2 per mg
0.049 for Ni, 0.036 for Cd and 0.031 for Mn. sample) (De Groot 2004). In order to optimize our re-
Out of the thirteen mineralized quartz samples from sults, we have used areas for analyses in the quartz sam-
the Agios Georgios veins, three were analyzed solely for ples examined under the microscope which primary fluid
δ18Ο at the Stable Isotope Research Laboratory, Univer- inclusions predominate. Silicon isotopes was measured
sity of Indiana, USA. The remaining ten samples were using the SiF4 technique of Ding (2004). Sulfur was re-
also analyzed for δ18Ο, δD and δ30Si at the Chinese Acad- leased as SO2 after the method of Fritz et al. (1974). The
emy of Geological Sciences, Beijing, China. A chalcocite isotopic ratios are reported in standard δ notation per mil
 8 E. Kevrekidis et al.

relative to SMOW for oxygen and hydrogen, NBS-28 for spar-plagioclase-quartz-magnetite, S-type leucogranite
silicon and CDT for sulfur. Analytical precision was bet- (Fig. 3a) , with dioritic enclaves (Table 3). The overall
ter than ± 0.2 per mil for δ18Ο, ± 1 per mil for δD, ± 0.1 per peraluminous character of the Paros leucogranite is also
mil for δ30Si and ± 0.2 per mil for δ34S. reflected in its accessory mineralogy of sillimanite, tour-
Lead isotopic compositions of four vein quartz sam- maline, Li-muscovite, apatite and garnet. The tectonic dis-
ples, representing sulfide grains in the veins, were deter- crimination diagram of Pearce et al. (1984) places the Pa-
mined at the Chinese Academy of Geological Sciences, ros leucogranite in the volcanic arc environment (Fig. 3b).
Beijing, China using an England Nu Plasma High Res- The amphibole (Table 3) is magnesio-hornblende and
olution Multi-Collector-Inductively Coupled Plasma- biotite (Table 4) plots near the phlogopite composition
Mass Spectrometer (MC-ICP-MS). Long-term repeated (Figs. 4a and 4b). The plagioclases have oligoclase to
measurements of lead isotopic ratios of standard NBS andesine and the alkali-felspars orthoclase compositions
981 yielded 206Pb/204Pb = 16.9397 ± 0.0111, 207Pb/204Pb (Table 5, Fig. 4c).
= 15.4974 ± 0.0089, and 208Pb/204Pb = 36.7147 ± 0.0262 The trends in major and trace element variations
(errors are reported at ± 2 σ). suggest the leucogranite magma evolved via fractional
Microthermometric measurements were obtained on crystallization of plagioclase (Figs. 5d, e, g, p and REE
doubly polished quartz wafers 50 –100 μm thick, using a profiles), amphibole (Fig. 5a, b, c, d, h, r), titaniferous
LINKAM MDSG600 heating-freezing stage coupled to a magnetite and ilmenite (Fig. 5a, c, h, j, l, m, r), apatite
ZEISS microscope in the Department of Earth Sciences (Fig. 5d, i), zircon (Fig. 5j) and probably allanite (Fig. 5a,
and Resources, China University of Geosciences, Beijing, d, g, q), and retention of biotite and alkali feldspar (Fig
China. Up to 30 inclusions were examined in each sam- 5e, f). The indicated kink in Nb concentration at 70 wt.%
ple. Temperatures were measured with an alumel-chromel SiO2 is attributed to uptaking of Nb in the zircon structure
thermocouple, and the readings were calibrated with syn- (Fig. 5l). The Paros leucogranite was emplaced at pres-
thetic inclusions at – 56.6 °C (triple point of CO2), 0.0 °C sures of 1.4 to 4.1 kbars or crustal depths of 4.1 to 8.8 km
(melting point of ice), and +374.1 °C (critical point of (Table 9) based on pressures calculated from the Altotal in
H2O). Measurements were accurate to within ± 0.1 °C and hornblende geobarometer (Schmidt 1992), which was ap-
freezing-heating rates were maintained between 0.2° and plied on ten different zoned hornblende crystals from the
5 °C/min. Microthermometric data were reduced using same thin section (Table 3). Depths were derived from
the software FLINCOR, for the system H2O-NaCl, em- these pressures based on the average lithostatic gradient
ploying the equations of Brown & Lamb (1989), Zhang & of 3 kbar/km. Application on the Ti-in-biotite (Table 4)
Frantz (1990) and Darling (1991). geothermometer of Henry et al. (2005) and the Al-in-
Fluid inclusion laser Raman spectroscopy analyses hornblende geothermo-barometer of Vyhnal et al. (1991)
were carried out in the Beijing Research Institute of Ura- utilizing the experimental calibrations of Schmidt (1992),
nium Geology, Beijing, China, using a Renishaw RM-
provided magmatic temperatures of 657° to 738 °C and
2000 Raman spectroscopy microscope. The same quartz
676° to 759 °C, respectively. Additionally, magnetite-il-
wafers prepared for microthermometry were also used for
menite pairs in the same thin section (Table 6) provided a
Raman analyses. The Raman work was done before heat-
similar spread of magmatic temperature values.
ing runs in order to avoid losses from decrepitation. The
The experimental work of Scaillet et al. (1995) ar-
instrument recorded peaks in the range of 100 – 4000 cm–1
gues that the leucogranite liquidus for these pressures is
full-band with a resolution of 1– 2 cm–1, and the laser beam
≤ 700 °C depending on the volatile content. The Paros
spot size was about 1 μm. The inclusions were analyzed
leucogranite magma was water saturated as shown by the
for the most common gases, monoatomic and polyatom-
presence of pegmatites and miarolitic cavities. For such
ic ions and molecules. Their relative concentrations (in
melts and at magmatic temperatures of ~700 °C the water
mol %) were calculated based on equations adopted from
content of the Paros leucogranite is estimated at 7 wt.%
Frezzotti et al. (2012) and the cross-sectional scattering
H2O following the methodology of Liu et al. (2005).
coefficients of Dhamelincourt (1979).
Therefore this is a granite rich in volatiles (-OH, B, F) a
composition reflected in its accessory mineralogy of Li-
Results rich muscovite, tourmaline and apatite which establishes
its potential for hydrothermal ore deposition. A summary
The leucogranite of Paros of the inferred conditions of emplacement of the Paros
leucogranite in given in Table 9. The distance of the Paros
The Miocene granitic intrusion of Paros is mainly a pluton from the Agios Georgios deposit is ~12 km, which
light grey hornblende-Li-rich muscovite-biotite-K feld- is comparable to the distance of 16 km between the Tinos
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 9

Fig. 5. Harker diagrams for major (wt.% ) and trace (ppm) elements. The trends (highlighted by hand-fit lines) are consistent with the evolu-
tion of the Paros leucogranite magmas via extensive crystal fractionation. See text for details.
 10 E. Kevrekidis et al.

Table 4. Microprobe single point chemical analyses of biotite from the leucogranite of Paros (from sample 1 of Table 1).
wt. %  1  2  3  4  5  6  7  8  9 10 11
SiO2 36.95 36.14 36.19 36.59 36.83 36.64 35.14 36.09 35.30 37.04 37.32
TiO2  3.71  3.43  3.51  3.63  3.48  3.44  3.65  3.62  3.50  3.49  2.97
Al2O3 13.94 13.62 13.83 14.02 13.76 13.44 13.47 13.93 13.11 13.66 13.69
FeO 16.03 16.55 16.94 16.00 16.19 16.31 16.31 16.66 16.31 16.12 16.08
MnO  0.57  0.54  0.53  0.59  0.63  0.57  0.55  0.50  0.52  0.57  0.66
MgO 13.94 12.75 13.43 13.88 14.04 13.36 13.04 13.67 12.67 14.00 14.52
CaO  0.04  0.22  0.05  0.01  0.07  0.06  0.14  0.07  0.15  0.03  0.04
Na2O  0.20  0.66  0.49  0.19  0.19  0.34  0.48  0.36  0.68  0.18  0.15
K2O  9.95  9.31  9.61  9.83  9.83  9.58  9.59  9.73  9.27 10.06 10.09
Cr2O3  0.15  0  0.01  0.22  0.15  0.02  0  0  0  0.17  0.13
Total 95.49 93.22 94.59 94.95 95.17 93.76 92.48 94.64 91.52 95.33 95.64
Number of ions on the basis of 24 oxygen atoms
Si  5.84  5.87  5.80  5.82  5.85  5.90  5.78  5.78  5.85  5.87  5.89
Al IV  2.16  2.13  2.20  2.19  2.16  2.10  2.23  2.22  2.15  2.13  2.11
Total  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00  8.00

Al VI  0.43  0.47  0.42  0.44  0.42  0.45  0.38  0.41  0.41  0.42  0.01
Ti  0.44  0.42  0.42  0.43  0.42  0.42  0.45  0.44  0.44  0.42  0.35
Fe2+  2.12  2.25  2.27  2.13  2.15  2.20  2.26  2.23  2.26  2.14  0.09
Mn  0.08  0.07  0.07  0.08  0.09  0.08  0.08  0.07  0.07  0.08  3.42
Mg  3.28  3.09  3.21  3.29  3.32  3.21  3.20  3.26  3.13  3.31  0.01
Ca  0.01  0.04  0.01  0  0.01  0.01  0.02  0.01  0.03  0.01  0.05
Na  0.06  0.21  0.15  0.06  0.06  0.11  0.15  0.11  0.22  0.06  0.05
K  2.01  1.93  1.97  1.99  1.99  1.97  2.01  1.99  1.96  2.03  2.03
Cr3+  0.02  0  0  0.03  0.02  0  0  0  0  0.02  0.02
Total  8.44  8.47  8.52  8.45  8.47  8.44  8.55  8.52  8.52  8.47  8.00

Table 5. Microprobe single point chemical analyses of feldspars Ore mineralogy and ore chemistry
from the leucogranite of Paros (from sample 1 of Table 1). Samples
1 to 5 are plagioclase and 6 is a K-feldspar.
Metallic and vein filling hydrothermal minerals formed
wt %  1  2  3  4  5  6 in three mineralizing Stages, two hypogene (I, II) and
SiO2 61.06 61.45 60.51 61.22 63.74 65.15 one supergene (III) (Table 10). High temperature ore
Al2O3 24.36 23.93 24.56 24.29 22.42 18.51 and gangue minerals (390° to 285 °C) such as chalco-
CaO  5.96  5.71  6.27  5.92  3.75  0.09 pyrite (Table 7), bornite, tetrahedrite, sphalerite, pyrite,
Na2O  7.79  7.95  7.58  8.03  9.45  2.30 pyrrhotite, and magnetite formed before closure of the
K2O  0.45  0.39  0.47  0.34  0.32 13.86
veins (Fig. 7). Euhedral pyrite (Table 8) contains up to
Total 99.62 99.42 99.38 99.80 99.67 99.90 0.67 wt.% As, 0.13 wt.% Zn and 0.14 wt.% Cu and sub-
Number of ions on the basis of 32 oxygen atoms hedral chalcopyrite up to 0.15 wt.% Zn (Table 7). Milky
Si 10.88 10.96 10.82 10.89 11.29 11.96 quartz is the main high temperature hydrothermal quartz
Al  5.11  5.03  5.17  5.09  4.68  4.00 being deposited together with calcite and ankerite during
Ca  1.14  1.09  1.20  1.13  0.71  0.02 the whole extent of Stage I. Epidote, sericite and chlorite
Na  2.69  2.75  2.63  2.77  3.25  0.82
also precipitated in Stage I.
K  0.10  0.09  0.11  0.08  0.07  3.25
Stage II ore minerals, including argentiferous ga-
Total 19.92 19.91 19.93 19.96 20.00 20.05
lena (Table 8), argentite, native Ag and Au formed after
re-opening of the hydrothermal conduits, i.e., after the
temperature interval of 245° to 130 °C (Fig. 7). The main
leucogranite and the Panormos Bay polymetallic Au-Ag gangue mineral of Stage II is clear hydrothermal quartz
telluride mineralization with which it is thought to be as- with lesser smithsonite (Table 10). Barite is ubiquitous in
sociated (Tombros et al. 2007, 2010). Stage II and probably denotes the localized inundation of
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 11

Table 6. Microprobe single point chemical analyses of magnetite from the leucogranite of Paros (from sample 1 of Table 1).
wt %   1  2  3  4   5  6   7   8   9 10
SiO2   0.04  0.02  0.05  0.05   0.05  0.10   0.04   0.02   0.03  0.06
TiO2   0.07  0.42  0.45  0.05   0.59  0.15   0.03   0.11   0.13  0.13
Al2O3   0.13  1.17  0.20  0.17   0.59  0.48   0.12   0.15   0.21  0.31
FeO  30.76 29.92 30.31 30.65  30.43 30.48  30.78  30.75  30.61 30.49
Fe2O3  68.36 66.50 67.37 68.13  67.65 67.75  68.41  68.35  68.04 67.76
Cr2O3   0.33  0.45  0.68  0.28   0.50  0.27   0.20   0.41   0.46  0.19
MnO   0.14  0.17  0.195  0.15   0.41  0.12   0.13   0.14   0.14  0.17
MgO   0.02  0.04  0.03  0.02   0.01  0.03   0.01   0   0  0.04
Nb2O5   0.01  0  0.04  0   0.03  0.01   0   0.03   0  0
ZnO   0  0.65  0  0.04   0.05  0.12   0   0.05   0.08  0.06
V2O3   0.33  0.32  0.36  0.35   0.28  0.30   0.31   0.38   0.37  0.03
Total 100.18 99.66 99.68 99.88 100.60 99.79 100.04 100.37 100.06 99.25
Number of ions on the basis of 32 oxygen atoms
Fe3+  15.82 15.39 15.66 15.80  15.55 15.70  15.85  15.79  15.76 15.80
Si   0.01  0.01  0.02  0.01   0.02  0.03   0.01   0.01   0.01  0.02
Ti   0.02  0.10  0.10  0.01   0.13  0.03   0.01   0.03   0.03  0.03
Al   0.05  0.42  0.07  0.06   0.21  0.17   0.04   0.05   0.07  0.11
Nb   0  0  0.01  0   0  0   0   0   0  0
V   0.08  0.08  0.09  0.09   0.07  0.07   0.08   0.09   0.09  0.01
Cr   0.07  0.10  0.15  0.06   0.11  0.06   0.04   0.09   0.10  0.04
Total  16.05 16.10 16.11 16.04  16.10 16.08  16.04  16.06  16.07 16.02

Fe2+   7.91  7.69  7.83  7.90   7.78  7.85   7.92   7.89   7.88  7.90
Mn   0.03  0.04  0.05  0.04   0.11  0.03   0.03   0.03   0.04  0.04
Mg   0.01  0.02  0.01  0.01   0  0.01   0.01   0   0  0.02
Zn   0  0.15  0  0.01   0.01  0.03   0   0.01   0.02  0.13
Total   7.95  7.90  7.89  7.96   7.90  7.92   7.96   7.94   7.93  7.98

Table 7. Microprobe single point chemical analyses of chalcopyrite from the metalliferous veins of Agios Georgios deposit, Antiparos
(same sample as in Table 8.).
wt %  1  2  3  4  5  6  7  8  9 10 11 12
Fe 30.1 30.06 30.28 29.74 30.76 30.45 30.34 30.29 30.06 29.93 30.54 29.81
Zn  0.06  0.05  0.06  0.06  0.10  0.04  0.15  0.09  0.04  0.09  0.02  0.02
Cu 34.31 34.32 34.25 35.05 33.70 33.99 34.00 34.45 34.57 34.71 34.28 34.53
Ni  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.01  0.00
Co  0.01  0.00  0.03  0.00  0.00  0.01  0.02  0.00  0.02  0.00  0.02  0.02
S 35.04 34.95 34.82 34.36 34.86 35.07 34.92 34.90 34.97 35.25 34.74 35.47
As  0.01  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.01  0.00
Total 99.54 99.38 99.44 99.21 99.42 99.56 99.42 99.73 99.66 99.98 99.62 99.84
Number of atoms
Fe  1.06  1.06  1.07  1.05  1.08  1.07  1.07  1.06  1.06  1.05  1.07  1.06
Zn  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00
Cu  0.94  0.94  0.93  0.95  0.92  0.92  0.93  0.99  0.94  0.95  0.93  0.94
Ni  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00
Co  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00
S  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00  2.00
As  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00  0.00
Total  4.00  4.00  4.00  4.00  4.00  4.00  4.00  4.00  4.00  4.00  4.00  4.00
 12 E. Kevrekidis et al.

Table 8. Microprobe single point chemical analyses of pyrite, Ag-galena and argentite from the metalliferous veins of Agios Georgios
deposit, Antiparos (same samples as in Table 7.).
wt % Pyrite Pyrite Pyrite Pyrite Pyrite Pyrite Galena Galena Galena Galena Argentite
Fe  46.88  46.77 46.53  46.03  46.22  46.72  0.02  0.05   0.01  0.05  0.03
Pb   0.00   0.00  0.00   0.00   0.00   0.00 83.51 84.54  86.00 86.15  0.25
Cu   0.07   0.07  0.09   0.10   0.14   0.09  0.09  0.19   0.19  0.28  3.24
Zn   0.00   0.02  0.02   0.02   0.13   0.03  0.00  0.00   0.00  0.00  0.00
Ag   0.00   0.00  0.00   0.00   0.00   0.00  2.90  1.17   0.26  0.17 82.19
Co   0.01   0.02  0.00   0.02   0.01   0.04  0.00  0.00   0.00  0.00  0.00
Ni   0.00   0.00  0.00   0.01   0.00   0.00  0.00  0.00   0.00  0.00  0.00
Sb   0.00   0.00  0.00   0.00   0.00   0.00  0.09  0.13   0.01  0.00  0.00
As   0.00   0.00  0.00   0.64   0.67   0.63  0.09  0.01   0.00  0.00  0.01
Te   0.00   0.00  0.00   0.00   0.00   0.00  0.01  0.03   1.19  1.66  0.89
S  53.43  53.30 52.81  53.80  53.39  53.04 13.25 13.83  12.49 11.67 12.52
Total 100.39 100.18 99.45 100.63 100.56 100.54 99.96 99.95 100.15 99.98 99.13
Number of atoms
Fe   1.00   1.00  1.00   1.00   1.00   1.00  0.00  0.01   0.00  0.00  0.00
Pb   1.00   1.00  1.00   1.00   1.00   1.00  0.94  0.96   0.99  0.98  0.00
Cu   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.01   0.01  0.02  0.13
Zn   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.00   0.00  0.00  0.00
Ag   0.00   0.00  0.00   0.00   0.00   0.00  0.06  0.03   0.00  0.00  1.87
Co   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.00   0.00  0.00  0.00
Ni   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.00   0.00  0.00  0.00
Sb   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.00   0.00  0.00  0.00
As   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.00   0.00  0.00  0.00
Te   0.00   0.00  0.00   0.00   0.00   0.00  0.00  0.00   0.02  0.03  0.02
S   2.00   2.00  2.00   2.00   2.00   2.00  1.00  1.00   0.98  0.97  0.98
Total   3.00   3.00  3.00   3.00   3.00   3.00  2.00  2.00   2.00  2.00  3.00

Table 9. Summary table of conditions of emplacement of Paros Fluid inclusions


Leucogranite.
Pressure Depth Temperature Water content
Fluid inclusion data were obtained from milky and clear
(kbars) (km) (°C) (wt.%) vein quartz (bands A and B, Table 11). Only primary inclu-
0.9  3.1 676.4 4.1 sions were used in the microthermometric study follow-
1.4  5.1 689.5 5.1 ing criteria established by Rhoedder (1984): (i) relatively
1.5  5.6 692.9 5.5 large size inclusions between 5 to 30 μm, (ii) inclusions
1.9  6.9 702.2 6.1 aligned parallel to the outer faces of the quartz crystals,
2.5  9.2 718.1 6.8
2.8 10.3 725.1 7.3 and (iii) inclusions yielding relatively high values of ho-
3.1 11.3 732.3 7.5 mogenization temperatures (Th). The criteria by which
3.5 13.0 744.0 8.2 inclusions were deemed secondary and were therefore
3.7 13.7 748.8 8.6 avoided are the following (Rhoedder 1984): (i) Occur-
4.1 15.2 758.9 8.8
rence within cracks of the crystals which extend into the
Pressure at level of emplacement of Paros pluton from the Al-in- exterior of the crystal and intersect its surface, and (ii)
hornblende barometer of Schmidt (1992) with an uncertainty of relatively low Th values of the secondary inclusions com-
± 0.6 kbars and amphibole data of Table 3. Temperatures calculated pared to the higher Th values of the primary ones.
from the pressure sensitive geothermometer of Vyhnal et al. (1991)
with an uncertainty of ± 75 °C.
At room temperature, three types of primary fluid
inclusions were identified (Fig. 6): (i) Type L-V and V-L
inclusions consisting of aqueous liquid+vapor with the
the system by sea-water (see Tombros et al. 2014). Box- liquid phase being dominant (80 vol.%). The majority
work textures in chalcopyrite indicate its supergene re- of inclusions have V/V+L ratios ≤ ~20 %, however some
placement by covellite, malachite, azurite and/or goethite present V/V+L ratios up to ~80 % (Fig. 6, Table 11), (ii)
(Stage III). Galena is replaced by anglesite and cerrusite, Type L-L-V inclusions consist of aqueous liquid+carbonic
whilst sphalerite is replaced by smithsonite and goethite. liquid+vapor and occur in milky quartz. Those rich in
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 13

CO2 have V/V+L ratios between ~ 60 % and ~80 % and and consist of aqueous liquid+vapor+daughter crystals
are ellipsoidal in shape and may host CO2 clathrates, (iii) (Fig. 6). The presence of halite or calcite daughter crystals
Type S-L-V inclusions have filling percentages of ~30 % is a rare occurrence within the inclusions. The secondary
fluid inclusions belong solely into the L-V category and
are considerably poorer in the gaseous phase.
Table 10. Ore Paragenesis and crustification banding of hydrother- Final ice melting temperatures for the V-L and L-V
mal minerals from Agios Georgios deposit, Antiparos. inclusions in milky and clear quartz range from –11.7°
Bands A B to – 3.1 °C and – 8.4° to – 2.9 °C, respectively. These val-
Mineral stages Stage I Stage II Stage IΙΙ ues correspond to salinities of 5.4 to 15.7 and from 4.8 to
A
T (°C) 391-275 245-131 ≤ 100
12.2 wt.% NaCl equivalent (Fig. 7, Table 11). The melting
temperatures of clathrate in and L-L-V inclusions are be-
Milky quartz ▃▃▃▃▃▃▃▃▃
Clear quartz ▃▃▃▃▃▃
tween 4.5 ° and 6.1 °C, which indicates salinities of 6.9
Epidote ▃ to 9.3 wt.% NaCl equivalent (Fig. 7, Table 11) using the
Sericite ▃ equation of Darling (1991). The homogenization temper-
Chlorite ▃ atures for L-V and V-L fluid inclusions in milky and clear
Calcite ▃▃ quartz are between 275° and 408 °C and 131° to 245 °C,
Ankerite ▃▃▃▃ respectively (Fig. 7, Table 11). The L-L-V fluid inclusions
Smithsonite ▃▃▃ ▃▃▃▃ homogenized to liquid between 347° and 408 °C, whereas
Barite ▃▃▃▃
the CO2 subphases homogenized to liquid or vapor be-
Fluorite ▃
Pyrite ▃▃▃
tween 30.5° and 32.1 °C. The halite dissolution tempera-
Pyrrhotite ▃ tures (Thhalite ≥ Th) have been used to calculate the salinity
Magnetite ▃ of the ore fluid. These temperatures were ~ 346 °C which
Sphalerite ▃▃▃▃ correspond to 30.5 wt.% NaCl equivalent (Lecumberri-
Chalcopyrite ▃▃ Sanchez et al. 2012). In order to constrain the density and
Bornite ▃ pressure of entrapment of the fluid we have applied the
Tetrahedrite ▃▃ software FLUIDS (Bakker 2012) on the H2O-NaCl-CO2
Galena ▃▃▃▃▃▃▃
system. Their densities range from 0.75 to 0.91 g/cm3, re-
Argentite ▃
Native Au ▃
spectively. The high porosity and abundance of vugs in
Native Ag ▃ the marbles, the brittle character of the mineralized frac-
Covellite ▃ ▃▃▃▃ tures and the open-space filling textures of clear quartz
Anglesite ▃▃▃ veins suggest that the trapping pressures were closer to
Cerussite ▃▃▃ the hydrostatic pressure. The pressures for the L-V and
Chalcocite- ▃▃▃▃ V-L and S-L-V inclusions vary from ~100 to 135 bars.
Digenite
Goethite ▃▃▃▃ As suggested by Rhoedder (1984) and Goldstein &
Malachite ▃▃▃▃ Reynolds (1994) no pressure correction was applied to
Azurite ▃▃▃▃ the homogenization temperatures because evidence for
Pyrolusite ▃▃▃▃ CO2-effervescence suggests that the fluid inclusions were
A  Temperatures obtained from fluid inclusions and various gase-
trapped along the CO2 solvus. Evidence for phase sepa-
ous- (e.g, H2S, CO2/H2S, CH4/CO2, CO2, H2 and CO2/N2) and ration includes the observed coexistence of L-L-V, L-V
liquid-phase geothermometers (e.g., adiabatic-Si, Na-Li and Na-K- and clathrate bearing inclusions along with L-V and V-L
Ca) (Tables 12 a and b).

Table 11. Fluid inclusion microthermometric measurement results from Agios Georgios deposit, Antiparos.
Sample Mineral N Phases Tmice Th Tmhalite/ Salinity
(°C) (°C) Tmclathate (wt. % NaCl equiv)
(°C)
AAG-3 Milky quartz (stage I) 23 L-V and V-L –11.7 to -3.3 275 to 400 – 5.4 to 15.7
AAG-3 Milky quartz (stage I)  3 L-L-V – 347 to 408 4.5 to 6.1 6.9 to 9.3
AAG-3 Milky quartz (stage I)  1 S-L-V –9.1 321 346 30.5
AAG-1 Clear quartz (stage II) 29 L-V –6.3 to -2.9 131 to 245 – 4.8 to 12.2

Abbreviation: Th = Homogenization temperature, Tm, ice = Final ice melt temperature and Tm = final salt melt temperature.
 14 E. Kevrekidis et al.

inclusion populations from one area of the crystal to an-


other (Fig. 6), and the large variations of salinities at equal
temperatures (e.g., at T ~320 °C the salinities range from
0.4 up to 30.5 wt.% NaCl equivalent, Fig. 7). These varia-
tions in salinity are characteristic of a hydrothermal boil-
ing event (Fig. 6). Field evidence for phase separation is
also given by the occurrence of the silicified, calcite bear-
ing hydrothermal breccias with acicular, colloform and
jigsaw-textures adjacent to the veins.

Raman laser analysis of fluid inclusions

Laser Raman analyses were obtained on six vapor-rich


fluid inclusions hosted in milky and clear quartz that have
been previously used for microthermometric determina-
tions. Raman analyses revealed that the gaseous phase of
the mineralizing fluid contained H2O, CO2, H2S, N2, CH4,
NH3, H2 and O2 (Table 12 a). The gaseous phase displays
logXCO2/XCH4, logXCO2/XN2, logXCO2/XH2O, logXO2/XH2O,
logXH2S/XN2 and logXCO2/H2S ratios ranging from 1.71 to
2.39, 1.91 to 3.05, –1.21 to – 0.68, – 3.64 to – 3.01, – 0.07
to 0.60 and 1.98 to 2.54, respectively (Table 12 a). Varia-
Fig. 6. a – Photomicrographs of primary fluid inclusions showing
tion of the logXCO2/XN2, logXCO2/XCH4 and logXCO2/XH2O
varying gas to liquid ratios characteristic of a boiling event. I. Gas ratios could be explained by degassing due to efferves-
rich fluid inclusion. II. Liquid rich fluid inclusion. III. CO2 clathrate cence.
enclosed within a liquid rich fluid inclusion. IV. Fluid inclusion of Raman spectra of the inclusion liquid phase indicated
liquid and gas. The arrow points directly to the edge of the clathrate. that it contained the cations Na+1, K+1, Mn+2, Ca+2 , Si+2,
V. Calcite daughter crystal enclosed within a solid(CaCO3)-liquid-
vapor fluid inclusion. The arrow points to the edge of a calcite Al+3 and traces of Ti+2, Li+1, B+3 and Cu+2, and the anions
crystal, b – Secondary gas rich fluid inclusions (I) aligned with the SO4 – 2 and CO3 – 2 (ranging from 0 to 215 ppm). The dom-
plane of a “healed” crack within the quartz crystal. inant cations are Ca+2, Na+1, K+1, Mn+2 and Si+2 (Table

Fig. 7. Liquid-vapor homogenization


temperature versus salinity plot showing
densities (g.cm– 3) in the vapour-saturated
NaCl-CO2-H2O system. Density (g/cm3)
contours regressed from data generated
by the equation of Darling (1991) using
the software FLUIDS (Bakker 2012). The
arrows denote the variation of salinities.
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 15

Table 12 a. Gaseous phase compositions (in mol %) of individual fluid inclusions and calculated content ratios from Agios Georgios de-
posit, Antiparos.
Sample Mineral CH4C CO2B, C H2O O2 N2 H2SA, B H2 logCO2 logCO2/ logCO2/ logCO2 logO2/
/N2 CH4 H2O /H2S H2O
AAG-3 Milky quartz n.d.  7.56 92.2 n.d. n.d. n.d. 0.24 – – – 1.09 –    –
AAG-3 Milky quartz n.d.  2.24 96.73 n.d. n.d. n.d. 1.03 – – – 1.64 –    –
AAG-3 Milky quartz 0.05 11.21 86.71 0.02 0.01 0.04 1.89 3.05 2.35 – 0.89 2.45 – 3.64
AAG-1 Clear quartz 0.11  5.68 92.65 0.09 0.07 0.06 1.34 1.91 1.71 – 1.21 1.98 – 3.01
AAG-1 Clear quartz 0.07 17.2 82.51 0.05 0.04 0.05 0.08 2.63 2.39 – 0.68 2.54 – 3.22

Abbreviation: n.d. = not detected.


In a sample obtained from milky quartz NH3 was detected up to 0.07. Also the logH2S/N2 were 0.6 for milky and = – 0.07 for clear quartz.
The temperature estimates used the geothermometers H2S- and CH4/CO2- of Giggenbach (1991), the CO2/H2S- of Nehring & D’Amore
(1984) and the CO2-, the H2- and the CO2/N2- of Arnórsson & Gunnlaugsson (1985). The calculated temperatures for stage I-milky quartz
range from 302° to 341 °C and for stage II-clear quartz from 209° to 236 °C.

Table 12 b. Liquid phase compositions (in ppm) of the same individual fluid inclusions and calculated content ratios from Agios Georgios
deposit, Antiparos.
Sample Mineral Si+2, A K+, C Al+3 B+3 Li+, B Ca+2, C Na+, B, C CO3 – 2 logNa+/ logK+/ logCa+2/ logLi+/
K+ Ca+2 Na+ Na+
AAG-3 Milky quartz 1020 103  96 72 6.5 134   11  0.4 – 0.97 – 0.11 – 0.11 – 0.23
AAG-3 Milky quartz 1370  88  76 n.d. n.d. 354  180  3.2 – 0.69 – 0.60 – 0.60    –
AAG-3 Milky quartz 1090  65  56 57 n.d. 105 1308 12.3 – 0.70 – 0.21 – 0.21    –
AAG-1 Clear quartz  670  20 n.d. n.d. n.d. 215  214 18.5    1.03 – 1.03 – 1.03    –
AAG-1 Clear quartz  950 250 174 69 1,7 192   13 24.6 – 0.28 – 0.89 – 0.89 – 0.88

In a sample obtained from milky and clear quartz were detected Li +1 and Mn2+of 6.5 and 1.7 and 75 and 89 ppm, respectively. Also in
milky quartz Ti2+ and Cu2+ and SO42 – were detected up to 1.3, 1.4 and 2.6 ppm, respectively.
We have used the adiabatic Si-A of Fournier & Potter (1982), the Na-LiB- of Fouillac & Michard (1981) and the Na-K-Ca geothermom-
eterC of Fournier & Truesdell (1973) for both milky and clear quartz. The log     Ca     + 2.06 values are positive and T ≥ 100 °C and so
Na
β = ¾.

12 b). The cation ratios logNa+1/K+1, logK+1/Ca+2, logK+1/ 345 °C. Stage II-clear quartz has deposited from 206° to
Mn+2and logLi+1/Na+1 for milky and clear quartz fluid in- 236 °C.
clusions range from – 0.97 to +1.03, –1.03 to +0.32, – 0.32
to +1.03, and – 0.89 and – 0.22, respectively. The logCa+2/
Mn+2 values were obtained only on clear quartz and range Isotopes
from – 0.87 to 0.46. Additionally, the logCO3 – 2/SO4 – 2 Oxygen, hydrogen and silicon isotopes
ratios in milky quartz are +0.33. The logNa+1/K+1 and
logK+1/Ca+2 ratios of the Antiparos ore fluid are identi- Oxygen and hydrogen isotope compositions were deter-
cal to the ones related to magmatic-dominated geothermal mined on the same samples of milky and clear vein quartz.
analogues (Giggenbach 1991). Also traces of Cu+2 and B+3 The δ18O values of milky quartz from band A range from
detected in the liquid phase support this hypothesis. 7.7 to 9.3 per mil. The measured δDH2O values from fluid
Based on the Raman results application on various gas- inclusion waters were – 61.2 to – 52.4 per mil (Table 13).
eous- (e.g., the H2S- and CH4/CO2- of Giggenbach 1991, Clear quartz veins (band B) display δ18O values of 6.5
the CO2/H2S- of Nehring & D’amore 1984 and the CO2-, to 12.1 per mil and δDH2O values from –73.2 to – 57.2 per
the H2- and the CO2/N2-geothermometers of Arnórsson mil. The corresponding δ18OH2O values of the ore fluids
& Gunnlaugsson 1985, Table 12 a) and liquid-phase geo- in equilibrium with milky quartz (based on temperatures
thermometers (e.g., the adiabatic Si- of Fournier & Pot- obtained from fluid inclusions, Table 11) range from 1.2 to
ter 1982, the Na-Li- of Fouillac & Michard (1981) and 2.8 per mil (Fig. 8). Also the δ18OH2O values of the miner-
the Na-K-Ca-geothermometer of Fournier & Truesdell alizing fluid in equilibrium with clear quartz range from
1973 (Table 12 b), has shown that stage I-milky quartz 5.4 to 11.6 per mil (Fig. 8). Lastly, a quartz sample of Pa-
has precipitated at temperatures ranging from 302° to ros leucogranite yielded δ18O values of 9.6 per mil. The
 16 E. Kevrekidis et al.

Table 13. Stable and lead isotope data from the vein quartz of Agios Georgios deposit, Antiparos.
Sample Mineral T1 δ18OV-SMOW δ18ΟΗ2Ο δDH2O δ30SiNBS-28 206Pb/204Pb 207Pb/204Pb 208Pb/204Pb

(°C) (per mil) (per mil) (per mil) (per mil)


AHK1 Milky quartz  310  9.3  2.8 – 71.8 – 0.5 18.805 15.604 38.543
AF11 Milky quartz  310  7.7  1.2 – 66.4 – 0.5 18.820 15.616 38.606
AF8 Milky quartz  310  7.9  1.4 – 64.4 – 0.4  –  –  –
AF8 Clear quartz 2051  6.9  5.8 – 66.7 – 0.6  –  –  –
AF8 Clear quartz  205  6.5  5.4 – 73.2 – 0.1  –  –  –
AHK9 Clear quartz  205 12.1 11.0 – 68.0    0.0 18.827 15.630 38.635
AHK8 Clear quartz  205 10.3  9.2 – 63.6 – 0.1 18.832 15.634 38.662
AHK1 Clear quartz  205 10.2  9.1 – 62.8 – 0.5  –  –  –
AF8 Clear quartz  205  6.9  5.8 – 66.6 – 0.2  –  –  –
AF11 Clear quartz  205  9.5  8.4 – 57.2 – 0.5  –  –  –
Paros Quartz  400  9.6  5.1 – 66.7    –  –  –  –
Leucogranite
AHK-9 Alteration zone quartz 12.6 11.6    – n.a.  –  –  –
AHK-3B Alteration zone quartz 11.8 10.8    – n.a.  –  –  –
AHK-1 Alteration zone quartz 10.3  9.3    – n.a.  –  –  –

(n.a.: Not analyzed)


1: Average temperatures obtained from fluid inclusion assemblages in milky and clear veins.

Fig. 8. Diagram of delta DH2O versus


delta 18OH2O per mil for the Antiparos
ore fluid. Samples plot in the fields of
magmatic and metamorphic waters,
which indicates mixing between the two
types of fluids as a result of wall-rock
interaction. The “Meteoric Water Line
(MWL)”, “Andesite and Subduction-
Related Vapor, Arc and Crystal Felsic
Magma (Magmatic Box)”, “Standard
Mean Ocean Water (SMOW)”, “Kao-
linite line” and “Metamorphic waters”
are also shown after Giggenbach (1992)
and Hedenquist & Lowenstern (1994).
The sample analyzed from Paros leu-
cogranite was obtained from Thapsana
site. Bands A and B contain milky and
clear quartz, respectively (Table 8).

corresponding δ18OH2O value of the ore fluids in equilib- position as all granites reported by Savage et al. (2012),
rium with Paros leucogranite was 5.0 per mil and δDH2O i.e., δ30SiNBS = – 0.23 ± 0.15 per mil.
values of – 66.7 per mil, at 400 °C (Table 13).
The obtained δ30SiNBS values of milky quartz veins are Lead isotopes
almost constant at – 0.5 to – 0.4 per mil (Fig. 9, Table 13).
Additionally, clear quartz veins display δ30SiNBS values Four whole rock lead isotope results were obtained from
which range from – 0.6 to 0.0 per mil (Table 13). The vein milky and clear quartz veins related to ore stages I and
quartz from Antiparos has the same silicon isotope com- II. Their 206Pb/204Pb, 207Pb/204Pb and 208Pb/204Pb ratios
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 17

Fig. 9. Diagram of 208Pb/204Pb versus


206
Pb/204Pb using age-corrected data.
The samples plot on the orogen line,
which is consistent with lead derived
from the Paros orogenic leucogranite.
The Lower and Upper Crust and Oro-
gene curves were based on the model
of Zartman & Doe 1981).

are displayed in Table 13. We also show previously pub- in the data probably reflects closure of the vein system due
lished data from Stos-Gale et al. (1996) for comparison. to precipitation of milky quartz (Fig. 7). This effectively
Based on the 206Pb/204Pb versus 207Pb/204Pb uranogenetic deterred hydrothermal fluid circulation and further depo-
and the 206Pb/204Pb versus 208Pb/204Pb thorogenic plots sition, thus no or very few fluid inclusions were trapped
it is apparent that a most plausible source for lead is an during this period. When the fluid reaches a temperature
orogenic-setting pluton, i.e., the Paros leucogranite rather of ~ 240 °C an increase of pressure within the vein system
than leaching of Pb from the upper crustal Hercynian met- resulted in fracturing and reopening of the hydrothermal
amorphic basement (Fig. 9).
conduits which allows once again the free circulation of
the hydrothermal fluid. The ensuing decrease in pressure
may have caused boiling of the hydrothermal fluid which
Discussion
together with mixing and cooling enhanced deposition
Origin and evolution of the metalliferous of clear quartz and argentiferous galena. This is the main
hydrothermal fluid mineralization event (Stage II), which together with the
preceding Stage I characterize the deposit as “epither-
The fluid inclusion temperature vs. salinity diagram mal”. Deposition of hydrothermal quartz, as clear quartz,
(Fig. 7) suggests mixing between a high temperature continued until the fluid reached a temperature of ~130 °C
and high salinity fluid (possibly juvenile, i.e. intrusion
as depicted from primary fluid inclusions.
related) and a low temperature, low salinity fluid. The
We estimated the partial pressures of dissolved gases
trend of fluid inclusion compositions offers a strong argu-
based the Herny’s law and the results of Raman analy-
ment for mixing with meteoric waters. Fluid inclusions
with considerably higher salinity, have the same trapping ses, adopting Henry’s law coefficients from Henley et al.
temperature as fluid inclusions with much lower salinity (1984). The partial pressures of CH4, CO2, H2O, O2, N2,
(Fig. 7). This suggests that CO2-effervescence occurred in H2S and H2 are estimated as 0 to 1.16, 7.8 to 94.6, 24.8 to
the fluid possibly due to wall-rock interaction (Tombros 29.02, 0 to 0.54, 0 to 0.1, 0.13 to 0.31 and 0 to 0.1 bars. The
et al. 2007). total pressures of the dissolved gases in the ore fluid range
The episode of the hydrothermal mineralization on from 38.3 to 120.8 bars (for milky and clear quartz veins),
Antiparos island begins with hydrothermal fluid at a tem- which correspond to a depth of phase separation varying
perature of ~ 400 °C. Between ~ 240° and ~ 290 °C, a gap from ~450 to 1600 m.
 18 E. Kevrekidis et al.

Table 14. Calculated physicochemical parameters of the hydrother-


mal fluids in stages I and II of Agios Georgios deposit, Antiparos1.
Parameter Stage I Stage II
Temperature (°C) 330 210
pH 3.6 to 4.0 5.4 to 5.5
logαSiO2(aq) –1.9 –2.4
logfS2 –8.6 to -7.3 –
logαH2S(g) –1.4 to -1.2 –
logαH2g) –1.09 to 0.28 –
logαH2S(aq) –3.78 to -3.13 –3.22 to -2.94
logαHS–(aq) –2.17 to -1.98 –2.21 to -1.94
logfCO2 –0.22 to -0.18 –0.13 to -0.09
logfO2 –31.3 to -32.4 –34.0
logαFe+2 –4.2 –
logαZn+2 –7.5 to -8.3 –
logαCu(HS)aq)–2 –7.6
logαAu(HS)2 –(aq) – –11.8
logαAg+ – –
logαPb+2 – –4.3 to -5.2
1Assuming mean temperatures for stages I and II of 330° and 210 °C

(milky and clear quartz), salinities of 4.8 to 13.1 wt percent NaCl


equivalent and pressures of 135 bars and ionic strength I = 0.18. See
text for details.

Physicochemical conditions of ore deposition

The physicochemical conditions of the Antiparos min-


eralization were estimated from phase stability relation-
ships using SUPCRT92 (Johnson et al. 1992) with ther-
modynamic properties from the 2007 database (slop07. Fig. 10. LogfO2 (in atm) versus pH isothermal diagram for: (a) Stage
dat; Shock 1998). These estimations were based on the I and (b) Stage II. Thicker dashed lines represent the stability field
coexistence among sulfides and silicates assuming Na- boundaries for pyrite (FeS2), pyrrhotite (FeS), hematite (Fe2O3) and
Cl-saturated aqueous liquids. Temperatures of 330° and magnetite (Fe3O4), at 330° and 210 °C, respectively. The Fe-S-O
mineral boundaries are shown for ΣS = 0.1 moles/kg H2O. Thin
210 °C are assumed to be representative of Stages I, and
short dashed and dashed-dotted lines are the calculated contours
II of the Antiparos ores. We have also assumed salinities for the sulfur and tellurium species in solution. Also shown are the
of 4.8 to 13.1 wt.% NaCl equivalent and pressures of 135 stability boundaries for kaolinite and K-mica (thin dotted line), and
bars. All solid phases were considered to have ideal solu- galena-anglesite (thin short dashed dotted line)
tion behavior. Individual ion activity coefficients of dis-
solved species were calculated using the B-gamma exten-
sion of Helgeson et al. (1981). The calculated values of The pH values were calculated from on the Raman-de-
ionic strength of ore solutions is I = 0.18 ± 0.1 termined composition of the fluid inclusions (at 330 °C,
The values of logαSiO2(aq) calculated from the equilibri- Stage I) and from the CO2 equilibrium (Reaction 2, Table
um of milky and clear quartz with the ore fluid (Reaction 14, Fig. 10a, b). For CO3 – 2 values which range from 0.4
1) are –1.9 and – 2.4, respectively. The fCO2 values were to 12.3 (milky quartz) and 18.5 to 24.6 ppm (clear quartz),
estimated by using the Henry’s law at the same tempera- the calculated logαCO3 – 2 values are – 0.39 to 1.09, and
tures and for Henry’s law constants obtained from El- 1.27 to 1.39 respectively. The obtained pH for Stages I
lis & Golding (1963). For the salinity range of the fluids and II range from 3.6 to 4.0 and 5.4 to 5.5, respectively
trapped in inclusions in milky and clear quartz, the values (Fig. 10a, b).
of logfCO2 are – 0.22 to – 0.18 and – 0.13 to – 0.09, respec-
5CuFeS2(s)+S2(g) = Cu5FeS4(s)+4FeS2(s) (3)
tively (Table 14).
CH4(g) +2H2O(g) = CO2(g)+4H2(g) (4)
SiO2(s)+2H2O(l) = 2H2O(l)+SiO2(aq) = H4SiO4(aq)(1)
CO2(g)+H2O(aq) = CO3– 2(aq)+2H+(aq)  (2) 2Η2S(aq)+O2(g) = S2(g)+2H2O(l)  (5)
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 19

H2S(g) = H2S(aq)  (6) Paros leucogranite: A probable source for the


mineralization fluids?
H2S(aq) = H+(aq) +HS–(aq)  (7)
Miocene plutons of the Cyclades in the back arc of the
0.5H2O(l)+ Au(ΗS)– 2(aq) = Au(s)+2HS–(aq)+H+(aq)+ Quaternary Aegean Arc are known to be related to hy-
0.25O2(g)  (8) drothermal mineralization events (Fig. 1) (Skarpelis 2007,
FeS2(s)+Η2O(l) = Fe+2(aq)+2ΗS–(aq)+0.5O2(g)  (9) Skarpelis & Argyraki 2009, Voudouris et al. 2008, Mas-
trakas 2007, ST. Seymour et al. 2009a, 2009b, Bonsall
ZnS(s)+H+(aq) = Zn+2(aq) +HS–(aq)(10) et al. 2011, Tombros et al. 2007, 2010, 2014). In this work
we have shown many lines of evidence suggesting that
CuFeS2(s)+Η2S(aq)+0.5H2O(g) = Cu(HS)2 –(aq)+ the Agios Georgios mineralization is related to the Paros
Fe+2(aq)+0.25O2(g)+ΗS–(aq) (11) S-type leucogranite.
PbS(s)+H+(aq) = Pb+2(aq)+HS–(aq) (12) Paros S-type granite magmas were emplaced at mid-
crustal depths (4 to 5 kbars), as dictated by the intersec-
The coexistence of pyrite, pyrrhotite-sphalerite-mag- tion of the muscovite breakdown curve with the water-
netite requires logfS2 values which range from – 8.6 to saturated granite solidus. Paros melts formed at relatively
–7.3 at T = 330 °C (Craig & Barton 1973). In the same low temperatures (~700 °C) and were rich in volatiles a
Stage the logfS2 values were mainly controlled by the characteristic typical of leucogranite melts. As such, they
equilibrium of pyrite ± bornite and chalcopyrite (Reac- crystallized not too far from the site of their generation.
tion 3). Based on this reaction the estimated logfS2 val- However, due to extensive crystal fractionation, incom-
patible trace elements were concentrated in the residual
ues were approximately at – 8.2. Additionally, the as-
melts (Fig. 5). Water saturation occurred also in the resid-
semblage of tetrahedrite and chalcopyrite for T = 330 °C
ual magmas by a second boiling event to form pegmatites.
yields a maximum logfS2 value of –7.7 (Craig & Barton
Li, B, F and P together with water in the residual magmas
1973).
depressed the temperature of the water-saturated solidus
Using the Raman data for the gaseous phase obtained
to lower temperatures (500° to 600 °C). Therefore, the
from fluid inclusions (Table 14) and the equilibria of the
Paros residual magmas continued their upward migration
gaseous phases CH4, CO2 and H2 (McCartney & Lanyon
to higher levels in the crust (at pressures of 100 to 135
1989; reaction 4, Table 14), we derived the actual logfO2
bars) and they would make prime candidates for the for-
values which vary from – 31.3 to – 32.4 (Stage I) and ~
mation of hydrothermal mineralization (as suggested also
– 34.0 (Stage II), respectively (Fig. 10a and b, Table 14).
by Strong 1981).
The latter values coincide with the appearance of galena To recapitulate then, extensive crystal fractionation
in Stage II at T = 210 °C and pH values of 5.4 to 5.5, which which is apparent from the Harker differentiation dia-
require maximum logfO2 values of – 34.2 (Craig & Bar- grams (Fig. 5) resulted in residual magmas rich in vola-
ton 1973). Utilizing the same data and the approach of
tiles such as H2O, P, Li, B, F and trace elements. This
McCartney & Lanyon (1989) (Table 14) we have calcu- is supported by the presence of apatite, Li-rich musco-
lated the logfH2S(g) and logfH2(g) values. The acquired val- vite and tourmaline in the accessory mineral assemblage
ues for Stage I range from ~ –1.4 to –1.2 and –1.09 to 0.28, (Kevrekidis 2013). The presence of abundant pegmatites
respectively. Values of logαH2S(aq) of ~ – 3.78 to – 3.13 and and miarolitic cavities additionally indicates that the Pa-
– 3.22 to – 2.94 and logαHS–aq) = – 2.17 to –1.98 and – 2.21 ros leucogranite magmas were water-saturated. For such
to –1.94, were determined from reactions 5, 6 and 7, for melts and at magmatic temperatures of 700 °C the water
Stages I and II respectively and for the logfO2, pH and content is ~7 wt.% (Liu et al. 2005). The Paros magma
logfS2 values calculated above (Table 14). ascended to 8.8 to 4 km, as is indicated by amphibole geo-
Finally, from the equilibria of reaction 8 concerning barometry, which corresponds to depths where the vol-
native gold precipitation at Stage II, the obtained value atile-depressed solidus is intercepted at 650 °C. Volatiles
of logαAu(HS)2 –(aq) was –11.8. Based on the reactions and incompatible elements would be expected then to be
involving pyrite, sphalerite, chalcopyrite and galena, concentrated in the Paros residual magmatic fluids, which
the logαFe++(aq), value was – 4.2 and the logαZn++(aq) at temperatures of 500° to 600 °C and after a second boil-
range from –7.5 to – 8.3 (reactions 9, 10, 11 and 12). The ing would continue their migration to shallow levels in the
logαCu(HS)2 –(aq) value was –7.6. The logαPb++(aq) ranged crust at pressures indicated by the primary fluid inclusion
from – 4.3 to – 5.2 (Table 14), (for pH = 3.6 to 5.5 and log- data. Structural control promoted fluid circulation. In the
fO2 = – 31.3 to – 34) (Stage II). case of the Paros leucogranite foliation and joints could
 20 E. Kevrekidis et al.

provide the necessary pathways for fluids as it becomes conclusions. The Agios Georgios mineralization event
apparent by the presence of quartz and pegmatites lit-par- was initiated at temperatures in excess of 400 °C based on
lit and cross-cutting veins which have been observed in fluid inclusion data, and the chain of mineralizing events
the field and of the Agios Georgios anticline resulting in can be described as follows:
the circulation and concentration of the metalliferous flu- 1) In the early stage the hydrothermal fluids with a pH of
ids in the area (Kevrekidis 2013, Evans & Fischer 2012 3.6 invaded marble host rocks in fractures in the hinge
and references therein). zone of the Agios Georgios anticline causing CO2 ef-
Substantial evidence for the predominantly magmatic fervescence which is indicated by the presence of CO2
origin of the Agios Georgios mineralizing fluids is de- clathrates and by Raman ratios i.e., log(CO2/CH4) and
rived from the stable isotope data. Magmatic values of log(CO2/H2O) in fluid inclusions in precipitating early
all granites for δ30SiNBS are – 0.23 ± 0.15 (Savage et al. milky quartz.
2012). The average value for the higher temperature milky 2) A sealing of the hydrothermal system in the tempera-
quartz of Antiparos is δ30Si = – 0.28 per mil with a range ture interval of ~240 to 290 °C, presumably due to quartz
from δ30Si = – 0.4 per mil and for clear quartz the aver- precipitation, is indicated by the gap in fluid inclusion
age δ30Si = – 0.34 per mil ranging between – 0.6 to 0.0. populations in this temperature interval.
However, the δ30Si values that are ≤ – 0.5 per mil may rep- 3) At temperatures below 240 °C, re-opening of the sys-
resent leached-out silicon derived from the CBU schists. tem presumably by fracturing and pressure release caused
The average sulphur isotopic value in Agios Georgios boiling of the fluid increase of the pH of the fluid and
chalcocites of δ34S =+4.1 ‰ is also well within the range deposition of clear quartz and argentiferous galena during
for magmatic sulphur (Seal 2006). The δ 18O values of the epithermal stage (240 –130 °C). The lower temperature
clear quartz and milky quartz yield calculated δ18OH2O fluids used the same conduits as the earlier ones and this
values of the hydrothermal fluid between +1.2 to +11.0 is displayed in veins where clear quartz tension gashes are
per mil, overlapping the magmatic range from ~+5 to +10 enveloped by milky quartz.
per mil (Hedenquist & Lowenstern 1994). From Fig. 8 it 4) The precipitation of the ore and accompanying miner-
becomes apparent that most of the clear quartz isotopic als was effectuated by T drop which was partly induced
values plot together with the Paros leucogranite within the by mixing with meteoric waters especially at the high end
“Magmatic Box”. Quartz samples from the alteration zone of the temperature spectrum.
around the veins plot mostly in the box of “Metamorphic The following lines of evidence point towards a coeval
Waters”, as expected due to wall-rock interaction. High- relationship between the Agios Georgios mineralization
temperature milky quartz samples plot between the mag- and the Paros pluton:
DD The pluton is a leucogranite rich in volatiles (-OH, F,
matic box and the “meteoric H2O” line. This can be ex-
plained by the fact that initially the plumbing system was B, P) and incompatible elements reflected in its ac-
more open and unarmoured, allowing fluids of magmatic cessory mineralogy of tourmaline, apatite and Li-rich
origin to mixing with meteoric waters. muscovite. Similar elements have been found in the
The alluded coeval relationship between the Paros leu- fluid inclusions in hydrothermal quartz by Raman
cogranite magma and the Antiparos mineralizing fluid is spectroscopy.
DD The stable isotope values of δ18O 34
consistent with many other results from this study. Fluid in- H2O, δD, δ SH2S and

clusion data reveal that mineralization was initiated at high δ30Si have close to magmatic values. Late clear quartz,
temperatures of ~ 400 °C. A magmatic contribution is sug- which was least mixed with meteoric waters since it
gested by the Raman evidence of Li, B and F in the hydro- was shielded by milky quartz veins, plots in the “mag-
thermal fluid (Table 12 b). Therefore, based on the grounds matic box” in a diagram of δ18OH2O versus δDH2O per
of the presented geological and geochemical arguments we mil.
DD Finally, the initial high temperature of the mineraliz-
suggest that the Paros leucogranite was the source for the
Agios Georgios, Antiparos mineralizing fluids. ing fluids (> 430 °C) supports the thesis that the source
of heat and ore fluid is the Paros pluton.

Conclusions
Acknowledgements
This study of hydrothermal mineralization in the quartz
vein-hosted argentiferous galena deposit at Agios Geor- We would like to thank Prof. Dr. Giannis Koukouvelas,
gios as well as of the composition and emplacement con- Prof. Dr. Sotirios Kokkalas and Dr. Dimitrios Spanos for
ditions of the Paros leucogranite reaches the following their invaluable suggestions and comments in the field of
The Agios Georgios argentiferous galena deposit on Antiparos Island, Cyclades, Hellas 21

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Manuscript received: July 18, 2014; accepted: March 11, 2015.


Responsible editor: R. Trumbull

Authors’ addresses:
Elias Kevrekidis (corresponding author), Department of Geology, University of Patras, Rion, Patras, 26504, Greece. e-mail: kevrekidis@
upatras.gr
Karen St. Seymour, Department of Geology, University of Patras, Rion, Patras, 26504, Greece: e-mail: kstseymr@upatras.gr
Stylianos Tombros, Department of Geology, University of Patras, Rion, Patras, 26504, Greece. e-mail: tombrosfs@gmail.com
Degao Zhai, State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, 100083, Beijing,
China. / School of Earth Sciences and Resources, China University of Geosciences, 100083, Beijing, China. e-mail: zhaidgcugb@gmail.
com
Jiajun Liu, State Key Laboratory of Geological Processes and Mineral Resources, China University of Geosciences, 100083, Beijing,
China. / School of Earth Sciences and Resources, China University of Geosciences, 100083, Beijing, China. e-mail: liujiajun@cugb.edu.
cn
Dimitrios Zouzias, Department of Geology, University of Patras, Rion, Patras, 26504, Greece. e-mail: dizouzias@gmail.com

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