The Laqiong Sb-Au deposit: Implications for polymetallic mineral systems in the Tethys-Himalayan zone of southern Tibet, China

Gondwana Research 72 (2019) 83–96

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The Laqiong Sb-Au deposit: Implications for polymetallic mineral systems in the Tethys-Himalayan zone of southern Tibet, China Hua-Wen Cao a, Hao Zou b,c,⁎, Leon Bagas d,e, Lin-Kui Zhang a, Zhi Zhang a, Zhong-Quan Li b a

Chengdu Centre, China Geological Survey, Chengdu, Sichuan 610081, China Key Laboratory of Tectonic Controls on Mineralisation and Hydrocarbon Accumulation of Ministry of Land and Resources, Chengdu University of Technology, Chengdu, Sichuan 610059, China State Key Laboratory of Lithospheric Evolution, Institute of Geology and Geophysics, Chinese Academy of Sciences, Beijing 100029, China d MLR Key Laboratory of Metallogeny and Mineral Assessment, Institute of Mineral Resources, CAGS, Beijing 100037, China e Centre of Exploration Targeting, The University of Western Australia, 35 Stirling Highway, CRAWLEY, WA 6009, Australia b c

a r t i c l e

i n f o

Article history: Received 7 November 2018 Received in revised form 18 February 2019 Accepted 25 February 2019 Available online 26 March 2019 Handling Editor: F. Pirajno Keywords: Laqiong Sb-Au deposit U-Pb zircon age Ar-Ar age C–H–O–Pb–S isotope Tethys-Himalayan zone

a b s t r a c t The Himalayan mineral field includes over 50 quartz-vein type Sb-Au deposits, and placer Au deposits. The poorly documented Laqiong deposit is a typical example of quartz-vein type Sb-Au mineralisation in Tethys Himalayan sequence. The orebody are controlled by shallow north-dipping normal faults and north–south trending faults. Magmatic zircons extracted from muscovitic leucocratic granite from the southern part of the Laqiong mine area yield a Laser Ablation-Inductively Coupled Plasma-Mass Spectrometry U-Pb age of 14 ± 1 Ma (n = 12, MSWD = 0.9) that is similar to the 40Ar/39Ar age of ca. 14 Ma from hydrothermal sericite in auriferous sulphide-quartz veins. The εHf(t) values for the magmatic zircon rims range from −5.4 to −1.9, corresponding to two-stage Hf model ages of 1403–1214 Ma. Quartz from the mineralised veins has δ18OH2O-SMOW values varying from +4.97 to +9.59‰ and δDH2O-SMOW values ranging from −119.7 to −108.1‰. The δ13CV-PDB values for calcite from the ore Stage III range from −6.9 to −5.3‰, and calcite from Stage IV are −3.5 to −1.7‰. The δ18OV-SMOW values for calcite from Stage III are +20.3 to +20.6‰ and for Stage IV are −6.3 to −4.9‰. The stibnite and pyrite samples have 208Pb/204Pb ratios of 38.158 to 39.02, 207Pb/204Pb ratios of 15.554 to 15.698, and 206 Pb/204Pb ratios of 17.819 to 18.681, and bulk and in-situ δ34SV-CDT values for stibnite, arsenopyrite and pyrite range from −1.1 to +2.3‰. The calcite from the orebodies are enriched in MREE and depleted in LREE and HREE. Fieldwork, petrological, and geochemical data collected during our study leads to the following salient findings: the mineralising fluid is a mix of magmatic and meteoric fluids; and the deposit is closely related to the emplacement of Miocene granites originating from a thickened continental crust. © 2019 International Association for Gondwana Research. Published by Elsevier B.V. All rights reserved.

1. Introduction The Tethys-Himalayan tectonic zone, also known as the TethysHimalayan foreland tectonic belt, is located between the Tibetan Plateau to the north and Indian Plate to the south (Fig. 1). The orogen is significantly mineralised and often referred to as the “global giant Himalayan metallogenic belt” (Schwartz et al., 1995; Pirajno, 2013 and references therein; Zheng et al., 2014; Hou and Zhang, 2015; Cao et al., 2016, 2017). The multi-metallic mineralisation includes the Cenozoic Au, Sb, Au-Sb, Pb–Zn–Ag, and W-Sn-Be deposits (Sun et al., 2016a). The Cenozoic Southern Tibet Sb-Au mineral field is in the Himalayan Orogen to the south of the Indus-Yarlung-Zhangbo Suture (IYZS) and to the north of the South Tibet Detachment zone (STD) (Fig. 1a). The orogen contains over 50 Au-Sb and placer-Au deposits (Fig. 1b) (Nie ⁎ Corresponding author at: College of Earth Sciences, Chengdu University of Technology, Chengdu, Sichuan 610059, China. E-mail address: [email protected] (H. Zou).

et al., 2005; Yang et al., 2009). Examples of deposits include the Chalapu, Zhemulang, Mayoumu, and Bangbu Au deposits, Laqiong and Mazhala Au-Sb deposits, and Cheqiongzhuobu, Zhegu and Shalagang Sb deposits (Yang et al., 2009; Li et al., 2002; Nie et al., 2005; Wen et al., 2006; Duo et al., 2009; Jiang et al., 2009; Zheng et al., 2014). Models proposed for these deposits include a variety of hydrothermal fluids derived from magmatic, mixed magmatic–meteoric sources in submarine exhalative, epithermal, or orogenic settings (Zhai et al., 2014; Zhang, 2012; Yang et al., 2009; Hou and Cook, 2009). We have selected the recently discovered Laqiong Sb-Au deposit in the southern part of the Tibet mineral field as a test area aiming to better define the regional tectonic setting for the mineralisation. The data presented here are based on systematic geological investigations, geochronological, isotopic geochemistry including new: (1) robust U-Pb zircon dates of granites and Ar-Ar dates of hydrothermal sericite to precisely document the ages of magma emplacement and Sb-Au mineralisation; (2) Lu-Hf isotopes of zircon to determine the genesis of the Laqiong leucocratic granite; and (3) H-O isotope data from quartz, C-O isotopes

https://doi.org/10.1016/j.gr.2019.02.010 1342-937X/© 2019 International Association for Gondwana Research. Published by Elsevier B.V. All rights reserved.

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Fig. 1. Geological maps showing: (a) tectonic divisions of the Qinghai-Tibet Plateau; and (b) location of Pb-Zn-Ag-Sb-Au polymetallic deposits in southern Tibet (Lin et al., 2016b). Abbreviations: THS = Tethys Himalayan Sequence, GHC = Greater Himalayan Crystalline Complex, LHS = Lesser Himalayan sequence.

data from calcite, Pb isotope data from stibnite and pyrite, bulk and insitu S isotope data from stibnite, arsenopyrite and pyrite, and the geochemistry of the calcite to constrain the source of the mineralising fluids. The results allow us to better understand the genetic relationship between mineralisation and magmatism, which are crucial for interpreting the geodynamics post the India–Eurasia continental collision.

2. Regional geology The Tethys-Himalayan Zone is located south of the IYZS and north of STD (Fig. 1a; Yin and Harrison, 2000; Yin et al., 2009; Pan et al., 2012; Zhang et al., 2012; Hu et al., 2015; Xu et al., 2015). The boundary between the Indian and Eurasian plates is marked by IYZS (Rowley, 1996, 1998; Zhu et al., 2005). The northward subduction of the Tethys oceanic plate is thought to have taken place during the Late Jurassic to Early Cretaceous at IYZS beneath the Lhasa Terrane, and closed in the Early Eocene with the collision between Indian Plate and Lhasa Terrane (Şengör et al., 1988; Zhu et al., 2013; Zhu et al., 2015; Hu et al., 2016; Najman et al., 2017).

The Tethys Himalayan sequence (THS) is located at the northern passive margin of the Indian Plate and consists of Precambrian to Early Palaeozoic orthogneiss (Zhang et al., 2019), widespread Mesozoic to Paleocene marine sedimentary units, and Eocene-Oligocene continental sedimentary rocks (Fig. 1b; Li et al., 2016; Zhang et al., 2015, 2016; Cai et al., 2016). The marine sedimentary units include low-grade sandstone, calcareous shale, siltstone and carbonate rocks, which host Cenozoic Pb-Zn, Au, Sb-Au and Sb deposits in the region (Yang et al., 2009; Wang et al., 2016; Pei et al., 2016; Sun et al., 2016a). The collision of the Indian and Eurasian continental plates resulted in the formation of the Tethys-Himalayan foreland tectonic zone (Qi et al., 2008). The zone includes complexly folded rocks with axial trends and associated brittle-ductile thrusts parallel to the orientation of the Tethys-Himalayan orogen. The STD is a large extensional tectonic zone between high-grade crystalline rocks in the Greater Himalayan Crystalline Complex and low grade THS, which are gently inclined northward, and played a major role in controlling the spatial distribution of deposits in the belt (Yang et al., 2009; Cottle et al., 2015; La Roche et al., 2016). The central part of THS contains a series of east-westward trending gneissic domes, also known as the north Himalayan gneiss domes (Fig. 1b; Zhang et al.,

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Fig. 2. Geology map of the Laqiong Sb-Au deposit in southern Tibet (a), and geological profile cross section of the deposit (b). Photographs of the ore-bearing veins at the No. I and II veis are shown in (c) and (d).

2012; Xu et al., 2013; Xu and Ma, 2015; Gao et al., 2016, 2017). Eocene and Miocene (ca. 48–8 Ma) dykes and stocks of leucogranites are present in the core of the domes (Zeng et al., 2011, 2015; Wu et al., 2015; Gou et al., 2016; Liu et al., 2016a, 2016b; Weinberg, 2016; Zhang et al., 2017; Zheng et al., 2016). The central and eastern part of THS contains large Early Cretaceous (ca. 135–130 Ma) bimodal igneous units consisting of basaltic lava, dolerite and gabbro, and minor amounts of ultramafic rocks and felsic dykes (Fig. 1b; Zhu et al., 2007, 2008, 2009; Liu et al., 2015; Ji et al., 2016).

3. Deposit geology The exposed units in the Laqiong mining area include the N100 m thick Early to Middle Jurassic Lure Formation, Middle Jurassic Zhela Formation, and Quaternary sediments (Fig. 2). The Lure Formation consists of grey to black carbonaceous calcareous shale and grey to white micritic limestone. The formation dips 10°–30° NNW and is unconformably overlain by the N500 m thick Zhela Formation in the mine area (Fig. 2b). The Zhela Formation consists of a metamorphosed succession

Table 1 Paragenetic sequence of minerals in the Laqiong Sb-Au deposit. Minerals

Stage I

Quartz Sericite Pyrite Stibnite Arsenopyrite Gold Chalcopyrite Cinnabar Calcite Dolomite Galena Jamesonite Chlorite Limonite Notes: major

minor

rare

.

Stage II

Stage III

Stage IV

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of grey to green, amygdaloidal basalt, basaltic andesite, purple tuff, grey siltstone, and grey micritic limestone, but the top of the formation is not exposed. The formation is widely exposed in the northern part of the mining area (Fig. 2a). The Middle Jurassic age of the formation is based on regional stratigraphic correlations and the presence of the Indocephalites sp., Dolikephalites sp., Reinekeia sp., and Garantiana sp. ammonite fossils (Xia and Liu, 1997; Zhu et al., 2004). Quaternary sediments are widely distributed in the region, and include diluvium along gullies, poorly sorted coarse-grained colluvium, eluvium, and locally present glacial till. The major structures in the Laqiong mining area include faults hosting the mineralised quartz veins locally called the No. I-, II- and III-veins (Fig. 2). The ore-bearing I-vein dips around 70–80° SW and

hosts most of the known Sb-Au mineralisation in the NW-SE trending Laqiong Fault. The fault is over 600 m long and the mineralised vein is in a 0.8–3 m wide and 120 m long breccia (Fig. 2c). The Sb-bearing No. II-vein is the second richest quartz vein in the area, and is hosted by a lenticular 2–5 m wide and 200 m long breccia zone developed in a N1200 m long reverse fault dipping ~60° northward (Fig. 2d). The Sb-Au(-Cu) mineralised No. III-vein is hosted by a NE-trending and NW-dipping sinistral fault that is about 500 m long, and up to 5 m wide. The mineralisation is in lenticular breccia containing disseminated pyrite, chalcopyrite and stibnite. Basalt, amygdaloidal basalt, andesitic basalt, trachybasalt, and ignimbrite assigned to the Zhela Formation are present to the north of the Laqiong Sb-Au deposit (Fig. 2a). Outcrops of leucocratic

Fig. 3. Photographs of ore and host rock alteration at the Laqiong Sb-Au deposit: (a) northward trending veins in the No. I orebody with a large amount of stibnite hosted by the Lure Formation; (b) strong alteration of the muscovitic Miocene leucogranite cut by a stibnite vein; (c) disseminated hydrothermal pyrite and arsenopyrite in strongly altered leucogranite; (d) stage II stibnite-quartz vein cutting a massive stage I vein; (e) paragenesis of Stage II minerals showing stibnite-quartz-calcite-pyrite-sericite; (f) stage II stibnite-quartz-calcite minerals; (g) stage III minerals represented by abundant quartz and minor stibnite; (h) cinnabar and limonite in the altered leucogranite; (i) massive stage IV calcite sampled from veins in the Lure formation; (j) photomicrograph of stibnite and quartz; (k) coexistence of stibnite and pyrite; (l) photomicrograph of arsenopyrite and quartz. Abbreviations: Apyarsenopyrite, Cal-calcite, Cin-cinnabar, Lm- limonite, Py-pyrite, Qtz-quartz, Ser-sericite, Stb-stibnite.

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Fig. 4. Photographs and diagrams of: (a) CL images of representative zircon grains; (b) zircon U-Pb Concordia diagrams and histograms of zircon 206Pb/238U ages for the muscovitic Laqiong leucogranite; (c) magmatic zircon U-Pb Concordia diagrams and weighted mean model ages for the muscovitic Laqiong leucogranite; and (d) inherited zircon U-Pb concordia diagrams and weighted mean model ages for the muscovitic Laqiong leucogranite.

muscovite-bearing granite are present south of the mining area, and intrude the Lure Formation around the mining area (Figs. 2a). The leucogranite is massive, and consists of quartz (40–45%), plagioclase (25–30%), K-feldspar (10–15%), muscovite (12–15%), biotite (3–4%), minor garnet (b1%), and accessory amounts of apatite and zircon.

Laqiong is a newly discovered low- to medium-grade deposit with grades between 1.04 and 74.55 g/t Au, and 0.5 to 13.77% Sb with a resource of at least 3000 kg Au and 5000 t Sb. The paragenesis of the hydrothermal mineral assemblages can be divided into four stages (Table 1). Stage I has simple mineral assemblage of quartz–sericite–

Fig. 5. Diagrams showing: (a) chondrite-normalised zircon REE patterns; (b) Ce/Ce* versus (Sm/La)N of zircon trace elements, where N indicated the assays are normalised to the chondrite values (after Hoskin, 2005); and (c) log10 Nb/Yb vs log10 U/Yb plot after Grimes et al. (2015) showing the origin of the magmatic zircon and inherited zircon grains of the Laqiong granite.

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Fig. 6. Diagrams for sericite from the auriferous sulphide-quartz veins from the Laqiong Sb-Au deposit: (a) 40Ar-39Ar plateau plot; and (b) isochron age plot.

pyrite, the Stage II assemblage contains the main Sb and Au mineralisation containing quartz–sericite–pyrite–stibnite– arsenopyrite–gold–chalcopyrite–galena–jamesonite. Stage III includes a small amount of sulphides with abundant calcite and quartz. Stage IV is characterised by calcite veins intruding the Lure Formation (Fig. 3).

dates between 188 and 169 Ma. Zircons with a weighted mean date of 174 ± 2 Ma (n = 14, MSWD = 0.98) are interpreted as inherited zircons from the Zhela Formation.

4. Samples and analytical methods

Zircon trace elements are sensitive monitors of the composition and temperature of their parental magma (Grimes et al., 2015). The trace element content of magmatic and inherited zircons from granite sample LQ-7 are listed in Supplementary Table 2. Magmatic zircons from the sample have a fractionated chondrite-normalised REE pattern indicated by strong positive Ce and negative Eu anomalies (Fig. 5a; Hoskin and Schaltegger, 2003; Whitehouse and Platt, 2003). The magmatic zircons' Th/U ratios are 1.2–2, Nb/Yb are 0.007–0.027, and U/Yb are 2.69–10.67. The U/Yb ratios are indicative of a continental setting (Fig. 5b–c, Grimes et al., 2015). The estimated temperature of zircon crystallisation using the Ti thermometry vary from at 740° to 809 °C (Watson et al., 2006; Ferry and Watson, 2007). The inherited Jurassic zircons have a fractionated chondrite-normalised REE pattern indicated by their positive Ce and negative Eu anomalies (Fig. 5a; Hoskin and Schaltegger, 2003; Whitehouse and Platt, 2003). The xenocrystic Jurassic zircons have

Twenty-two representative samples were collected from underground workings and outcrops in the Laqiong area (around 91°16′54″ E and 28°27′47″N) for various analyses. Sample LQ-7 is from a strongly altered leucogranite collected for zircon U-Pb, Lu-Hf isotope and trace elements analysis, and Sample LQ-24 is from an ore-bearing vein collected for sericite Ar-Ar dating. The other samples comprise six sulphide quartz veins for H-O isotope analysis, six calcite veins for C-O and bulk trace elements analysis, six stibnite and two pyrite samples for bulk SPb isotopes analysis, and ten spots on stibnite, arsenopyrite and pyrite analysed in-situ for S-isotopes. Detailed experimental procedures and data are presented in Appendix A, the zircon U-Pb dating analyses are listed in Table S1, zircon trace element data are given in Table S2, the Lu-Hf isotope data is presented in Table S3, the sericite Ar-Ar data are documented in Table S4, Quartz H-O data are shown in Table S5, calcite C-O data are presented in Table S6, the Pb and S analytical data from sulphides are listed in Tables S7 and S8, and trace element analytical results of calcite are presented in Table S9.

5.2. Zircon trace elements

5. Analytical results 5.1. Zircon U-Pb ages The zircon U-Pb isotopic data of the leucocratic muscovite granite are shown in Supplementary Table 1. Representative CL images of the zircons from sample LQ-7 are shown in Fig. 4a. All the zircons are euhedral in shape and have clear oscillatory zoning. All the Th/U ratios are between 0.3 and 2, which indicates a magmatic origin (Supplementary Table 2; Belousova et al., 2002). A total of 27 spots were analysed on 27 zircon grains. Twelve spots from magmatic zircons form a tight cluster on the Concordia curve, yielding concordant 206Pb/238U ages from 13 to 14 Ma with a weighted mean age of 14 ± 1 Ma (n = 12, MSWD = 0.93; Fig. 4b, c), which is interpreted as the crystallisation age of the muscovite-bearing leucocratic granite. Except for one spot on an inherited zircon yielding a date of ca. 130 Ma, 14 spots on inherited zircons form a tight cluster on the concordia curve in Fig. 4(b, d) yielding concordant 206Pb/238U

Fig. 7. Chondrite-normalised REE patterns of calcite from the Laqiong deposit. Normalised data are from McDonough and Sun (1995).

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Fig. 8. Diagrams showing: (a) histogram of ages for leucogranite in the Himalayan Orogen and the metallogenic age of Pb-Zn-Ag, Sb-Au and Au deposits in the Himalayas; and (b) zircon εHf (t) vs U-Pb ages of the muscovitic Laqiong leucogranite. For comparison, the fields of zircon Hf isotope compositions from Himalayas leucogranite are outlined (data from Lin et al., 2016a; Liu, et al., 2014; Wang et al., 2017; Zeng et al., 2015). Leucogranite age data from Nie et al., 2006; Qi et al., 2008; Gao et al., 2009, 2013; Yu et al., 2011; Huang et al., 2013; Harrison et al., 1997; Ding et al., 2005; Zeng et al., 2009; Lin et al., 2016b and this study. The geochronological date for mineral deposits are from Xie et al., 2017; Liang et al., 2015; Sun et al., 2016b; Pei et al., 2016; Lin et al., 2016b and this study).

relative high Th/U ratios range from 0.4 to 0.7, low Nb/Yb ratios of 0.002–0.006, and U/Yb ratios of 0.3–1.7 (Supplementary Table 2). The inherited zircons' estimated temperature of crystallisation using the Ti thermometry vary from at 642° to 876 °C (Watson et al., 2006; Ferry and Watson, 2007).

(t) values of inherited zircons were calculated based on each inherited zircon U-Pb age of ca. 174 Ma. The analytical results show that these zircons also have homogenous Hf isotopic compositions, with εHf(t) values of 6.7–10.9 that correspond to two-stage Hf TDM2 ages of 791–520 Ma, suggesting that the magma was derived from a juvenile Neoproterozoic crustal source.

5.3. Zircon Lu-Hf isotopes 5.4. Sericite 40Ar/39Ar ages Some of the zircons were also analysed for Lu-Hf isotopes on domains with the same or similar structure as those that were analysed for U-Pb isotopes. Eleven spots were analysed on magmatic zircons and 9 spots on inherited zircons (Supplementary Table 3). The results show that the magmatic zircons have relatively high 176Hf/177Hf ratios of 0.28261–0.28271 and low 176Lu/177Hf ratios of 0.000675–0.002032, and the high 176Hf/177Hf ratios are interpreted to represent the Hf isotope composition of the magma during magmatic zircon crystallisation (Amelin et al., 2000). The initial 176Hf/177Hf ratios and εHf(t) values of the magmatic zircon were calculated based on each magmatic zircon U-Pb age (ca. 14 Ma). The analytical results show that these magmatic grains have homogenous Hf isotopic compositions, with εHf(t) values that range from −5.4 to −1.9, which correspond to two-stage Hf model ages (TDM2) of 1403–1214 Ma, indicating that the magma was derived from Mesoproterozoic crustal sources. The initial 176Hf/177Hf ratios and εHf

The 40Ar-39Ar analytical results for sericite sample LQ-24 from the auriferous sulphide-quartz veins are presented in Supplementary Table 4 and illustrated in Fig. 6. The 40Ar-39Ar steps for sericite from the auriferous sulphide-quartz veins yield a plateau age of ca. 14 Ma based on 99.24% of the released 39Ar isotope, which were calculated from steps 1–7 (Fig. 6a). Regressing the most radiogenic steps through the composition of atmospheric argon (initial 40Ar/36Ar = 309.2 ± 10.7) on an isochrone diagram yields an age of 14 ± 1 Ma (MSWD = 1.93; Fig. 6b). This shows that the hydrothermal fluid and granite have a concordant age of ca. 14 Ma. 5.5. Stable isotopic (C–H–O–Pb–S) compositions The δ18OH2O-SMOW and δDH2O-SMOW values of quartz from stages II and III are similar and listed in Supplementary Table 5. The δ18OH2O-

Fig. 9. Diagrams showing: (a) the hydrogen vs oxygen isotope compositions for the Laqiong deposit (modified after Taylor, 1974); and (b) carbon vs oxygen isotope composition of the Laqiong deposit (modified from Taylor, 1974). The H-O isotope compositions from the mineral deposits in THS are from Meng et al. (2008); Zhang (2012), Mo et al. (2013), Yang et al. (2009), Du et al. (2013), Jiang et al., (2009), Zhou et al. (2011), Sun et al. (2010), Sun et al. (2013), Sun et al. (2016b), Pei et al. (2016). Data of Tibet hot water from Zheng et al. (1982). The C-O isotope compositions from the mineral deposits in THS are from Zhang et al. (2010), Meng et al. (2008), Yang et al. (2009). C-O isotopic data for mantle, marine carbonate rocks and sedimentary organic matters are sourced from Demény et al. (1998), Veizer and Hoefs (1976) and Hoefs (2009 and references therein).

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Fig. 10. Diagrams: (a) Y/Ho vs La/Ho plot for calcite from the Laqiong deposit (modified after Bau and Dulski, 1995); and (b) Tb/Ca vs Tb/La plot for calcite from the Laqiong deposit (Möller et al., 1976).

values vary from +4.97 to +9.59‰ and δDH2O-SMOW values range from −119.7 to −108.1‰. The C and O isotopic data for the calcite from the orebodies are listed in Supplementary Table 6. The δ13CV-PDB values are between −6.9 and – 5.3‰ for calcite from Stage III and –3.5 to −1.7‰ for calcite from Stage SMOW

IV, and the δ18O V-SMOW values are from +20.3 to +20.6‰ for the Stage III and –6.3 to −4.9‰ for the Stage IV. The Pb isotopic ratios for the six stibnite and two pyrite samples are 208 Pb/204Pb = 38.158 to 39.028, 207Pb/204Pb = 15.554 to 15.698 and 206 Pb/204Pb = 17.819 to 18.681 (Supplementary Table 7). Stibnite,

Fig. 11. Lead isotope diagrams for sulphides from the Laqiong deposit: (a) evolution curve of 207Pb/204Pb vs 206Pb/204Pb; (b) 208Pb/204Pb vs 206Pb/204Pb; (c) 207Pb/204Pb vs 206Pb/204Pb discrimination plot; and (d) 208Pb/204Pb vs 206Pb/204Pb plot for stibnite and pyrite (after Zartman and Doe, 1981). The available Pb isotope compositions for sulphide minerals and sediments are from Zhang et al. (2010), Sun et al. (2016b), Du et al. (2011), Jiang et al. (2009), Pei et al. (2016), Zhang (2012), Awang et al. (2017), Miào et al. (2017). Abbreviations: OIV - Oceanic island volcanic rocks; A - MORB; B/OR - Orogen; C/UC - Upper Crust; D/LC - Lower Crust.

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arsenopyrite and pyrite are the most common sulphides in the Laqiong mining area. The absence of sulphate minerals indicates that the δ34S value of the sulphides generally represents the δ34S∑S-fluids value of the hydrothermal fluids (Ohmoto, 1972). The δ34SV-CDT data from the six bulk stibnite samples range from −1.1 to −0.6‰, and the two bulk pyrite samples range from +1.5 to +1.7‰ (Supplementary Table 8). The in-situ δ34S values from the sulphide minerals range from +0.2 to +2.3‰, with of which stibnite ranging from +1 to +2.3‰, arsenopyrite from +1 to +1.3‰, and pyrite from +0.2 to +1.3‰. A characteristic is that their δ34S values decrease gradually from the core to the rim, such as in stibnite decreasing from +2.3 to +1.1‰ and pyrite decreasing from +1.3 to +0.2‰.

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5.6. Bulk trace element analysis Trace elements and REE analytical results from the calcite samples are documented in Supplementary Table 9. The trace element are relatively enriched in the large ion lithophile elements, such as Ba and Sr, depleted in the high field strength elements, such as Nb, Ta, Zr, Hf and Th, and have relatively high Y assays. The ΣREE (excluding Y) ranges from 5.44 to 17.39 ppm, with enrichment in MREE and depleted in LREE and HREE. The ΣLREE/ΣHREE ratio ranges from 1.11 to 2.96, (La/ Yb)N ratio ranges from 0.96 to 3.71, and with positive Eu anomalies (δEu between 1.19 and 2.05) and negative and slightly positive Ce anomalies (δCe values of 0.6 to 1.03) (Fig. 7).

Fig. 12. Diagrams: (a) comparison of in-situ and bulk S isotopic compositions of sulphide minerals at the Laqiong deposit; (b) histogram of in-situ and bulk S isotopic data from the Laqiong deposit; (c) comparison of the S isotope composition derived from the mantle, seawater, and evaporates (Heyl et al., 1974; Zou et al., 2017) and data from the nearby Pb-Zn-Ag-Sb-Au deposits in THS sourced from Zhang et al. (2010), Yang et al. (2006), Yang et al. (2009), Sun et al. (2016b), Du et al. (2011), Jiang et al. (2009), Pei et al. (2016), Zhang (2012), Awang et al. (2017).

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6. Discussion

2015; Harrison et al., 1999; Zhang et al., 2005; Guo and Wilson, 2012; Gao and Zeng, 2014).

6.1. Petrogenesis of granites 6.2. Formation of metallic ore 6.1.1. Age of granites Many chronological studies have been carried out in recent years revealing that the Himalayan leucogranite plutons range between ca. 48 and 8 Ma (Fig. 8a, Schärer et al., 1984; Edwards and Harrison, 1997; Coleman and Hodges, 1995; Harrison et al., 1999; Murphy and Harrison, 1999; Schneider et al., 1999; Simpson et al., 2000; Searle and Godin, 2003; Cottle et al., 2007; Kellett and Godin, 2009; Leloup et al., 2010; Sachan et al., 2010; Zhang et al., 2012). The age of leucocratic muscovite granite in Laqiong mining area is ca. 14 Ma, which is within the age range of the Himalayan leucogranite plutons in the region. There is no documentation of ca. 174 Ma magmatism in the region, but we know that mafic and intermediate volcanic units interbedded with fossiliferous sedimentary rocks of this age are present at the bottom of the Middle Jurassic Zhela Formation. Furthermore, ca. 130 Ma inherited zircons are similar in age to the Comei-Bunbury Large Igneous Province located between China, India, Australia, and Antarctica before breakup of Gondwana (Zhu et al., 2009).

6.1.2. Origin of granites The leucocratic muscovite granite in the Laqiong mining area is severely altered, and for this reason it has not been analysed for whole rock geochemistry. The granite is included in the famous northern Himalayan leucogranitic belt in THS (Fig. 1), which is characterised leucogranites with high aluminium saturation indexes (A/CNK N 1.1) containing minerals such as muscovite, garnet and tourmaline, are silicon-rich (SiO2 N 67%), and have low iron and magnesium contents (b5%), which are features characteristic of peraluminous granites (Lin et al., 2016a). The plutons commonly form batholiths or stocks derived from melting of the crust, and the presence of muscovite has been interpreted as being indicative of “S-type” granites sourced from pelitic rocks (Gou et al., 2016; Lin et al., 2016a; Hopkinson et al., 2017; Huang et al., 2017). The muscovitic Laqiong granite has negative magmatic zircon εHf (t) values of −5.4 to −1.9 indicating derivation from a Mesoproterozoic continental source. The εHf(t) of the Himalayan leucogranites also have negative values (Fig. 8b, Lin et al., 2016a; Liu et al., 2014; Zeng et al., 2015). These characteristics of the granites have been interpreted as evidence for derivation from partial melting of a metasedimentary source in a thickened continental crust (Knesel and Davidson, 2002; Zeng et al.,

6.2.1. Timing of mineralisation The age of mineralisation is an important criterion in determining the tectonic setting for its deposition and whether it is coeval with a magmatic event (Leach et al., 1998; Sun et al., 2013; Zou et al., 2019). The age of the Pb-Zn-Ag-Sb–Au mineralisation in THS has not been well determined due to the lack of suitable minerals for dating (Yang et al., 2009). In recent years, several mineralisation events have been recognised (Fig. 8a). Examples include the Zhaxikang Pb-Zn-Sb deposit dated at ca. 20 Ma by Xie et al. (2017) and ca. 12 Ma by Liang et al. (2015), Bangbu Au deposit dated at ca. 45 Ma by Sun et al. (2016b) and ca. 50 Ma by Pei et al. (2016), and Keyue Pb-Zn-Sb deposit dated at ca. 21 Ma by Lin et al. (2016b). Sericite collected from the auriferous sulphide-quartz veins at Laqiong yield a 40Ar-39Ar age of ca. 14 Ma (Fig. 6), which is supported by a LA-ICP-MS zircon U-Pb age of ca. 14 Ma for magmatic zircons from the leucocratic muscovite granite (Fig. 3). Detail regional and district geological field studies can also be used to constrain the timing of mineralisation, especially the recognition of tectonic events and associated structures controlling orebodies in THS. At least two kinds of faults controlling Sb, Sb-Au and Au deposits have been recognised. One set includes east–trending low-angle faults dipping northwards associated with STD (Hou and Cook, 2009). The STD's-related extension is constrained in age between ca. 20 and 15 Ma (Iaccarino et al., 2017). The second set includes northwardtrending normal faults located across the Himalayan–Tibetan Orogen (Fig. 1). Normal faults cutting STD are dated at ca. 8 Ma in the Himalayas, but are N14 Ma elsewhere in Tibet (Chen and Liu, 1996; Blisniuk et al., 2001). The geochronological data from Xainza–Dinggye rift show that the E–W extension began ca. 13 Ma, and remained active until ca. 8 Ma (Zhang et al., 2012). The intersection points between the northtrending normal faults and east-trending detachment faults commonly host mineralisation. This indicates that the mineralisation in THS formed in the period between 20 and 8 Ma. 6.2.2. Source of the ore-forming fluids Microthermometric data from Sb-Au deposits in southern Tibet, such as at Shalagang and Mazhala, indicate that the ore-forming fluids had low salinities at low temperatures (Zhang, 2012; Yang et al., 2006; Du et al., 2013). The absence of daughter-minerals in fluid

Fig. 13. Sketch cross-section of the collisional zone between the Indian and Eurasian plates, showing the tectonic setting for the Laqiong mineral deposits (from Grujic et al., 2011). Dashed line—assumed displacement path of mafic granulite and eclogite. The isoresistivity contours suggest a progressively higher fluid content in the core. Seismic bright spots that indicate zones with high fluid content were interpreted as putative magma chambers. Abbreviations: THS = Tethys Himalayan Sequence, GHC = Greater Himalayan Crystalline Complex, LHS = Lesser Himalayan Sequence. STD-South Tibet Detachment system; HHT-High Himalayan Thrust; MCT-Main Central Thrust; MBT-Main Boundary Thrust; MHT-Main Himalayan Thrust.

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inclusions hosted by gangue quartz and calcite rules out a direct orthomagmatic source for the mineralised fluids (Yang et al., 2009). This is significantly different from the high-temperature and highsalinity mineralised fluids associated with the Miocene Gangdese porphyry and skarn deposits. The δ18OH2O-SMOW and δDH2O-SMOW values in quartz from the Laqiong deposit are derived by applying the isotope fractionation equation by Clayton et al. (1972), which plot in the same area in Fig. 9a as defined by earlier analyses of Pb-Zn-Ag-Sb-Au deposits (cf. Taylor, 1974; Kong et al., 2015, and references therein). The δD values of −119 to −108.1‰ and δ18O values of +4.97 to +9.59‰ from Laqiong deposit are lower than those of metamorphic, mantle-derived, or magmatic fluids (Fig. 9a). In addition, the H-O isotopic values have a narrow distribution between the ranges of primary magmatic and meteoric water (Fig. 9a). We therefore conclude that the ore-forming fluids of Laqiong deposit originated from a mixed source of magmatic and meteoric fluid (Zou et al., 2016). Calcite separates have higher δ13CPDB values of −6.9 to −5.3‰ for the fourth hydrothermal stage (Stage IV) and −3.5 to −1.7‰ for Stage III which are higher than those of organic matter and lower than marine carbonate, but similar to those of magmatic- and mantle-derived fluids. These data indicate that magmatic intrusions may have contributed a significant proportion of carbon into the hydrothermal fluids (c.f. Ohmoto, 1972; Liu et al., 2007; Swain et al., 2015, and references therein). The δ 18 O SMOW values determined from the calcite separated from Stage III and IV veins are distinctly different, with values of +20.3 to +20.6‰ for Stage III and −6.3 to −4.9‰ for Stage IV, and both are lower than those of sedimentary organic matter (+22 to +30‰), and different from oxygen derived from the mantle (+2 to +7‰) and magma (+4 to +12‰) (Liu et al., 2007; Swain et al., 2015). The δ18O SMOW values for calcite from Stage IV plot close to meteoric water and calcite from Stage III plot in low temperature altered field of magmatic fluid in Fig. 9b. These results indicate that the ore-forming fluids for Stage III are not derived purely from magmatic intrusions, but are probably derived from a mixed source involving meteoric water, and the Stage IV calcite is derived from meteoric water formed after the main sulphide minerals stages II and III. The REE contents are commonly “tracers” for the geochemical behaviour of rocks, therefore the Y/Ho ratio is usually used to trace fluid processes (Bau and Dulski, 1995). The Chondrite-normalised REE patterns of calcite from stages III and IV shown in Fig. 7 are distinctly different indicating that they have different sources. This is also indicated by the C-O isotopic data and trace elements (Figs. 9b and 10). The Y/Ho and La/Ho values for calcite from the same source should be similar, and the ratio between them should be close to a straight line in the Y/Ho vs La/ Ho plot (Bau and Dulski, 1995). The calcite Y/Ho and La/Ho values of homologous non-synchronous crystallisation should display a negative correlation where the La/Ho ratios of recrystallised calcite have small variations. The Stge III Calcite samples have La/Ho ratios of 4.1 to 9 and Y/Ho ratios of 38.5–40.9; and the Stage IV calcite has significantly different La/Ho ratios of 1.5–2.5 and Y/Ho ratios of 46.1–58.9. Calcite from the deposit do not plot on a straight line in the Y/Ho vs La/Ho diagram shown in Fig. 10a, which is characteristic of distinct origins for the calcite from the two hydrothermal stages (c.f. Bau and Dulski, 1995). This is also confirmed by the contrasting C-O isotope compositions (Fig. 9b). The differences indicate that calcite veins in Stage IV are probably derived from the carbonate units in the Lure Formation, and have been affected by mineralised hydrothermal fluids resulting in a decrease in La/Ho and an increase in Tb/La values (Fig. 10). Möller et al. (1976) present the Tb/Ca vs Tb/La plot as a discrimination diagram representing the source of calcite according to its sedimentary, hydrothermal, and pegmatitic affinities (Fig. 10b). Six calcite samples from the Laqiong deposit plot in the hydrothermal field and one on the line between the hydrothermal and sedimentary fields indicative of a hydrothermal origin (Fig. 10b).

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6.2.3. Sources of the ore-forming materials The value of Pb isotopes are the most direct and effective method for tracing the source of ore-forming material, assuming they are not affected by radioactive decay and mixing, and do not vary during physical, chemical, and biological processes, and Pb isotopes remain unchanged during mineral migration and precipitation (Shen, 1987). These Pb isotopes are, therefore, used widely in the study of various types of deposits (e.g. Carr et al., 1995; Muchez et al., 2005; Zhou et al., 2013). The samples from the Laqiong deposit have high 208Pb/204Pb values of around 39, high 207Pb/204Pb values between 15.6 and 15.7, and high 206 Pb/204Pb values between 17.8 and 18.7. The Pb isotopic data plot in the Pb evolution curve and discrimination diagram predominantly in the upper crustal and orogene zones (Fig. 11; Zartman and Doe, 1981). In addition, the Pb-Zn-Ag-Sb-Au deposits in THS have similar Pb isotopic compositions, and are consistent with derivation from a Himalayan substrate (Fig. 11a, b). This might be due to the migration of sedimentary and magmatic material into ore-forming fluids forming a similar Pb isotopic composition as the host rocks (Zhang et al., 2010). Primary ore in Laqiong deposit consists of the assemblage stibnite– galena–sulphides, but lacks sulphate minerals. Hence, the δ34S values of the sulphides approximate those of the corresponding fluids (i.e. δ34S sulphide ≈ δ34S fluid; Ohmoto, 1972; Seal, 2006). The in situ δ34S values for sulphide minerals obtained range from +0.2 to +2.3‰, compared to the bulk sample analyses of −1.1 to +1.7‰ (Fig. 12a, b). These S-isotopic signatures are similar to magma-derived sulphur with δ34S values of −3 to 3‰ (Chaussidon et al., 1989), and consistent with a magma source for many Sb-Au deposits in THS (Ohmoto, 1979; Yang et al., 2009). Exceptions are the Zhaxikang and Keyue deposits with higher δ34S values characteristic of sulphur derived from rocks deposited in a marine environment (Fig. 12c; Zhang et al., 2010, Yang et al., 2006, Yang et al., 2009; Sun et al., 2016b; Awang et al., 2017). 6.3. Tectonic implications The Tethyan Himalayan tectonic belt is the product of the crustalscale shortening and thickening caused by subduction of the Tethyan oceanic plate followed by the collision of the Indian and Eurasian continents during ca. 65–55 Ma resulting in the formation of an eastward trending Himalayan orogen (Mo et al., 2007; Yin, 2006). The collision was accompanied by the formation of large-scale thrust faults, nappe structures, folds and the development of the east-trending STD and north-trending normal faults in THS. The high-grade Greater Himalayan Crystalline Complex from the middle and lower crust was exposed between by the Main Central Thrust to the south and STD to the north during the Neo-Himalayan tectonic event (Fig. 13; Patel et al., 1993; Hodges, 2000; Wiesmayr and Grasemann, 2002; Yin, 2000). The region cooled during ca. 15–13 Ma in response to a rapid tectonic exhumation by movement on late extensional structures at higher structural levels resulting in the emplacement of late leucogranite plutons (Vannay and Hodges, 1996). The Miocene magmatic activity resulted in a sharp increase in the geothermal gradient accompanied by widespread convection of groundwater along permeable zones such as the east-trending STD or north-trending normal faults. Hydrothermal fluids circulating around cooling magmatic bodies mixed with meteoric water. The degree of mixing was not the same around every magmatic body resulting in variations in the geochemistry of individual deposits deposited in dilational zones that were periodically closed and opened forming laminar, veins and lenticular Pb-Zn-Ag-Sb–Au orebodies in THS. 7. Conclusions The magmatic zircons from the leucocratic muscovite granite yield a U-Pb age of ca. 14 Ma (n = 12, MSWD = 0.93), and hydrothermal sericite from the auriferous sulphide-quartz veins yields an Ar-Ar age of ca. 14 Ma (MSWD = 1.93) in Laqiong Sb-Au deposit. These data

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suggest a close temporal relationship between magmatism and mineralisation. Magmatic zircons from the ca. 14 Ma muscovitic Laqiong leucogranite have negative εHf(t) values of −5.4 to −1.9, interpreted as being derived from the partial melting of a thickened Mesoproterozoic continental crust. The H-O and C-O isotopic data from the Laqiong deposit suggest that the fluid is a mixed magmatic and meteoric fluid. The bulk Pb isotopic data indicate that the source is from the upper crust associated with orogens. Both in-situ and bulk S isotopic data are characteristic of a deep magmatic source. In conclusion, the Sb-Au mineralisation at the Laqiong deposit is closely related to a Miocene leucogranite emplaced in a thickened crust.

Acknowledgements This study is financially supported by the National Key R&D Program of China (2016YFC0600308 and 2018YFC0604103), National Natural Science Foundation of China (41702108, 41802095, 41672196, 41741004), China Scholarship Council (201608515058) and Major cultivating project of Education Department of Sichuan Province (2018CZ0009). Appendix A. Supplementary data Supplementary data to this article can be found online at https://doi. org/10.1016/j.gr.2019.02.010.

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