Spatiotemporal reconstruction of Late Mesozoic silicic large ...

Spatiotemporal reconstruction of Late Mesozoic siliciclarge igneous province and related epithermalmineralization in South China: Insights fromthe Zhilingtou volcanic-intrusive complexGuo-Guang Wang1, Pei Ni1, Chao Zhao1, Xiao-Lei Wang1, Pengfei Li2, Hui Chen1, An-Dong Zhu1, andLi Li1

1State Key Laboratory for Mineral Deposits Research, Institute of Geo-Fluids, School of Earth Sciences and Engineering,Nanjing University, Nanjing, China, 2Department of Earth Sciences, University of Hong Kong, Hong Kong, China

Abstract Silicic large igneous provinces (SLIPs) generally reflect large-scale melting of lower crustalmaterials and represent significant metal reservoirs. The South China Block-Coastal Region (SCB-CR) SLIPhosts several large epithermal deposits. To better understand these deposits, we document thespatiotemporal framework of the host SLIP across the SCB-CR. Using zircon U-Pb dating and geochemical andisotopic analysis, we identify four stages of emplacement. Stage 1 felsophyre (circa 149Ma) shows a chemicalaffinity to highly fractionated I-type granites. Stages 2 and 3 of low-Mg felsic volcanics (circa 128 to 111Ma)and stage 4 felsite (circa 100Ma) have higher εHf(t) and εNd(t) values than stage 1 felsophyre, suggesting asignificant contribution of newly underplated juvenile crust to the magma sources. Stage 4 diabase (circa101Ma) was likely produced bymelting of subduction˗metasomatized asthenospheric mantle. Together withreliable published data, we build a new spatiotemporal framework of volcanics and infer that the majority ofthe SCB-CR SLIP was related to the gradual northwestward subduction of the Izanagi plate beneath SouthChina in a continental arc setting during circa 170 to 110Ma, and minor contribution was from the eastwardretreat of the subducting slab in a back-arc setting during circa 110 to 90Ma. We conclude that thelarge-scale epithermal mineralization was generated by melting of the metal-rich, thin (30–40 km), newlyunderplated hydrous juvenile crust during the tectonic transition from arc to back-arc settings.

1. Introduction

Mafic large igneous provinces (LIPs) are characterized by short-lived (<5Ma), large volume (>100,000 km3)mafic-ultramafic rocks in intraplate settings [Bryan and Ernst, 2008; Coffin and Eldholm, 1994; Ernst andBuchan, 2003]. In contrast to classic mafic LIPs, silicic large igneous provinces (SLIPs) are defined by (1) extru-sive volumes of> 10,000 km3 dacitic to rhyolitic ignimbrites; (2) emplaced over relatively long time intervals(generally> 20Ma); and (3) spatially/temporally associated with volcanic rifted margins or failed continentalrifts [Bryan, 2007; Bryan et al., 2002]. Examples include the Jurassic Chon Aike province and related rocks in therift zone of West Antarctica [Pankhurst et al., 1998], the Early Cretaceous Whitsunday igneous province in thevolcanic rifted margin of eastern Australia [Bryan et al., 1997], and the Oligocene to Early Miocene SierraMadre Occidental province in the Basin and Range extensional regime of western Mexico [Camprubi et al.,2003; Ferrari and Rosas-Elguera, 2002]. These well-known SLIPs are reported to have formed in back-arc exten-sional regimes associated with accreted continental margins or intraplate rifts [Bryan, 2007; Bryan et al., 1997;Ferrari and Rosas-Elguera, 2002]. In contrast, SLIPs generated in continental arc settings are not well studied.

The South China Block (SCB) is characterized by the widespread development of Late Mesozoic granitoids,diorites, gabbros, and their volcanic counterparts (Figure 1a). Additionally, over 90% of these magmaticrocks are granitoids and equivalent volcanic rocks with minor basalts [Zhou et al., 2006]. The SCB is alsofamous for the Qing-Hang Cu-Au-Pb-Zn-Ag porphyry-skarn metallogenic belt, the Nanling W-Sn-Nb-Taquartz vein and granite-related metallogenic belt, and the Coastal Region epithermal Au-Ag-Cu-Pb-Znmetallogenic belt [Ni et al., 2015; Pirajno and Bagas, 2002; So et al., 1998; G. G.Wang et al., 2015a; Zhaoet al., 2013]. Considering the great geological and economic significance of this region, the tectonic set-ting of the SCB during Late Mesozoic has attracted considerable attention but remains highly debated[Gilder et al., 1996; Hsü et al., 1988; Li and Li, 2007; Sun et al., 2007; G. G. Wang et al., 2015a; Xie et al.,

WANG ET AL. SLIP AND EPITHERMAL MINERALIZATION 7903

PUBLICATIONSJournal of Geophysical Research: Solid Earth

RESEARCH ARTICLE10.1002/2016JB013060

Key Points:• A Late Mesozoic northwestward andsubsequent eastward migration of theSouth China SLIP emplacementsequence is established

• The SLIP formed in an arc andsubsequent back-arc setting relatedto a northwestward subduction andfollowing slab retreat

• Epithermal mineralization formed bymelting of metal-rich juvenile crust inresponse to tectonic transition fromarc to back-arc regimes

Supporting Information:• Supporting Information S1

Correspondence to:P. Ni,[email protected]

Citation:Wang, G.-G., P. Ni, C. Zhao, X.-L. Wang,P. Li, H. Chen, A.-D. Zhu, and L. Li (2016),Spatiotemporal reconstruction of LateMesozoic silicic large igneous provinceand related epithermal mineralization inSouth China: Insights from theZhilingtou volcanic-intrusive complex,J. Geophys. Res. Solid Earth, 121,7903–7928, doi:10.1002/2016JB013060.

Received 6 APR 2016Accepted 18 OCT 2016Accepted article online 19 OCT 2016Published online 14 NOV 2016

©2016. American Geophysical Union.All Rights Reserved.

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http://dx.doi.org/10.1002/2016JB013060

http://dx.doi.org/10.1002/2016JB013060

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Figure 1. (a) Sketch map showing the Late Mesozoic volcanic-intrusive complex belt in South China [after G. G. Wang et al., 2012], ZJ = Zhejiang, FJ = Fujian,GD = Guangdong, JX = Jiangxi, HN = Hunan, HB = Hubei, GX = Guangxi, GZ = Guizhou, and AH = Anhui; (b) simplified geological map of the Zhilingtou igneousrocks and associated mineralization.

Journal of Geophysical Research: Solid Earth 10.1002/2016JB013060


1996; Xie et al., 2001; Zhou et al., 2006]. At least three competing tectonic models have been proposed,including a collision model [Hsü et al., 1988], a mantle plume model [Xie et al., 1996; Xie et al., 2001],and a paleo-Pacific (or Izanagi) plate subduction model [Li and Li, 2007; Sun et al., 2007; Zhou et al.,2006]. Hsü et al. [1988] reported the collision model and stressed the Late Mesozoic assemblage betweenthe Yangtze and Cathaysia blocks, but an increasing number of observations have revealed that the amal-gamation between these two blocks occurred during Neoproterozoic instead of Late Mesozoic [Zhaoet al., 2013; Zheng et al., 2008]. Xie et al. [1996] and Xie et al. [2001] proposed the mantle plume modelto explain the Late Mesozoic granitic magmatism in South China. However, mantle plumes generallyresult in the rapid formation of flood basalts [Stein and Hofmann, 1994; Tarduno et al., 1991] that areabsent in the SCB [Q. Liu et al., 2012b; Zhou et al., 2006]. Given obvious drawbacks of the above men-tioned two models, most researchers tend to agree with the paleo-Pacific plate subduction model[Jiang et al., 2015; Li and Li, 2007; Sun et al., 2007; G.G. Wang et al., 2015a; Zhou et al., 2006]. Thepaleo-Pacific subduction model remains hotly debated regarding the initiation time and drifting directionsof the paleo-Pacific plate. The subduction initiation time of the paleo-Pacific plate remains controversial,involving three different views: Li and Li [2007] proposed that the subduction started in the Late Permianand an intraplate setting developed in Yanshanian period; Jiang et al. [2015] argued that the subductionstarted in the Early Jurassic and then repeated advances and retreats of the slab occurred beneath theSouth China Block; Zhou et al. [2006] and Sun et al. [2007] proposed that the subduction of the paleo-Pacific plate beneath the SCB initiated in the Middle Jurassic. Finally, two different drifting directions ofthe paleo-Pacific plate were proposed. Sun et al. [2007] argued that the pacific plate drifted southwest-ward before circa 125Ma instead of northwestward as proposed by Zhou et al. [2006], Li and Li [2007],and Jiang et al. [2015].

Volcanic rocks are widely distributed in Zhejiang, Fujian, and Guangdong provinces in the South China Block-Coastal Region (SCB-CR) and cover an area of 100,000 km2. Given that more than 95% magmatic rocks arefelsic in composition, theymay constitute the SCB-CR SLIP [Wang and Zhou, 2005]. Recently, numerous robustzircon U-Pb dating results have suggested that the volcanics in Fujian and Guangdong provinces wereerupted between the Late Jurassic and the Late Cretaceous (circa 168 to 95Ma) [Guo et al., 2012; Liu et al.,2015]. In addition, some reliable zircon U-Pb dating data were obtained from volcanics in northern and south-eastern Zhejiang province and yielded ages of circa 140 to 88Ma [L. Liu et al., 2012a]. Voluminous felsic vol-canics in southwestern Zhejiang province crop out and constitute an important part of the SCB-CR SLIP, butno robust ages have been obtained from the volcanics in this region to date. It is crucial to clarify whether thefelsic volcanics in southwestern Zhejiang province formed between the Middle and the Late Jurassic, as pro-posed by the Bureau of Geology and Mineral Resources of Zhejiang Province [1989] or the Early Cretaceous simi-lar to the felsic volcanics in other regions of Zhejiang province [L. Liu et al., 2012a]. Moreover, the combinationof recently obtained reliable dating results from volcanics can provide a clear spatiotemporal framework ofthe SCB-CR SLIP and deeper insights into its tectonic evolution.

Epithermal deposits, first proposed by Lindgren [1933], are important sources of gold, silver, and base metalsand form at shallow crustal levels (<1.5 km) and at low temperatures (<300°C) [Robb, 2005; Simmons et al.,2005]. Epithermal deposits are generally hosted by coeval or slightly older volcanic rocks. Orebodies occurin veins with steep dips that formed through dilation and extension [Simmons et al., 2005]. Such hydrother-mal systems commonly develop in continental arc, intra-arc, back-arc, and intraplate rift settings [Sillitoe andHedenquist, 2003]. SLIPs have great economic significances and are closely linked with large-scale epithermalmineralization. The Sierra Madre Occidental SLIP in western Mexico was reported to host more than 800 EarlyMiocene (circa 24 to 20Ma) epithermal Au-Ag deposits or occurrences [Camprubi et al., 2003]. The SCB-CRSLIP is also characterized by the widespread occurrence of epithermal Au-Ag deposits such as theZijinshan, Wuziqilong, Yueyang, Dongyang, Qiucun, Taihuashan, Zhilingtou, Babaoshan, Wubu, andDalingkou deposits [Pirajno and Bagas, 2002; Zhong et al., 2014], but the links between SLIP and large-scaleepithermal mineralization remain unclear.

Studies on the Zhilingtou volcanic and intrusive complex are of great significance because this complexbelongs to a suite of voluminous felsic volcanics in southwestern Zhejiang province. This complex lacksrobust dating constraints and hosts the largest Au-Ag deposit in Zhejiang province [The No. 7 Team of theZhejiang Bureau of Geology and Mineral Resources, 2006]. In this contribution, we first conducted systematicLA-ICP-MS zircon U-Pb geochronology as well as elemental and Sr-Nd-Hf isotopic analyses to investigate



Figure 2. Typical filed and photomicrographs of four-stage Zhilingtou igneous rocks, including (a and b) stage 1 felsophyre,(c and d) stage 2 rhyolite, (e and f) stage 3 dacite, (g and h) stage 4 diabase, and (i and j) stage 4 felsite. Abbreviations:Pl, plagioclase; Kfs, alkaline feldspar; Aug, augite; Qz, quartz.



Table

1.ASu

mmaryof

theFu

ndam

entalR

esultsof

theZh

iling

touVo

lcan

ic-In

trusiveCom

plex

Stag

eRo

ckType

FieldOccurrence

Age

s(M

a)Elem

entsMajor

(wt%)M

inor

(ppm

)Sr-NdIsotop

esZircon

HfIsotop

esSampleLo

catio

n

1Felsop

hyre

Intrud

ingBa

duba

semen

tstrata

149

SiO277

.09–

77.34;K 2O5.60

–6.02;

P 2O50.01

–0.02;TiO20.12

–0.13;

Rb22

6–30

2;Zr,183

–212

;Ba46

–74;

Sr17

–31;Eu

0.05

–0.13

initial

87Sr/86Sr=0.70

3;ε N

d(t)=

�5.2;T

DM2=1.36

Ga

ε Hf(t)=

�18.6~�1

4.0;

T DM2=2.08

–2.36Ga

ZLT055

(long

itude

:119

°25

′41.5″,latitu

de:28°

36′42.5″);ZL

T054

-057

near-ZLT05

52

Rhyo

lites

Thelower

partof

theMoshishan

Group

128

SiO267

.92–

76.11;K 2O4.04

–6.22;

Rb11

1–33

1;MgO

0.20

–1.43;

Al 2O3mostly

<12

.71;Sr

11–1

40;

Mg#

25–3

7;Sr/Y

0.47

–12.27

initial

87Sr/86Sr=0.71

2–0.71

4;ε N

d(t)=

�6.6;T

DM2=1.46

Ga

ε Hf(t)=

�13.5~�1

.8;

T DM2=1.30

–2.02Ga

ZLT199

(long

itude

:119

°25

′36.4″,latitu

de:28°

37′14.8″);ZL

T201

-212

near

toZL

T199

;ZL

T259

(long

itude

:11

9°25

′48.1″,latitu

de:

28°37′23

.3″);Z

LT23

7-24

1ne

arto

ZLT259

3Dacite

sTh

eup

perpa

rtof

theMoshishan

Group

111

SiO264

.46–

70.20;Al 2O313

.92–

16.28;

Sr23

7–47

3;K 2O3.00

–5.78;MgO

0.42

–1.05;

Mg#

28–3

5;Sr/Y

9.84

–18.91

initial

87Sr/86Sr=0.71

1–0.71

4;ε N

d(t)=

�7.6~�5

.8;

T DM2=1.38

–1.53Ga

ε Hf(t)=

�11.5~�3

.6;

T DM2=1.39

–1.89Ga

ZLT065

(long

itude

:119

°25

′48.9″,latitu

de:28°

37′24.2″);ZL

T172

-176

from

38exploration

lineun

dergroun

dtunn

elat

420m

level;

ZLT276

-280

from

3841

unde

rgroun

dtunn

elat

380m

level

4Felsite

Cuttin

gvo

lcan

ics

ofthe

Moshishan

Group

100

SiO274

.98–

76.87;K 2O3.96

5.68

;CaO

0.24

–1.20;MgO

0.09

–0.26;P 2O5<0.01

;Nb11

.3–1

3.8;Ti52

7–68

6;Sr

82–1

57;

Ba43

4–60

5;Mg16

–36

initial

87Sr/86Sr=0.70

9–0.71

2;ε N

d(t)=

�0.6~+0.2;

T DM2=0.89

–0.95Ga

ε Hf(t)=

�8.1~�2

.2;

T DM2=1.30

–1.67Ga

ZLT006

-010

from

unde

rgroun

dtunn

elalon

gV-1orebo

dyat

180m

level;ZL

T137

-13

8from

unde

rgroun

dtunn

elalon

gV-2orebo

dyat

180m

level

Diaba

se10

1SiO244

.91–

47.11;K 2O2.63

–3.12;

Na 2O3.14

–3.43;MgO

4.37

5.59

;Ba

477–

2182

;Sr58

6–24

76;M

g#44

–55;

Nb13

.5–1

5.5;Ta

0.75

–0.89;Ti81

6–90

77

initial

87Sr/86Sr=0.70

7–0.70

8;ε N

d(t)=

�5.0~�2

.2;

T DM2=1.08

–1.31Ga

ε Hf(t)=

�5.0;T

DM2=1.48

Ga

ZLT001

-004

from

unde

rgroun

dtunn

elalon

gV-1oreb

odyat

180m

level



the petrogenesis of the Zhilingtou igneous rocks. Together with recently published work on the SCB-CR SLIP[Guo et al., 2012; Li et al., 2014; Liu et al., 2015; L. Liu et al., 2012a], we aim to reconstruct the spatiotemporalframework of the SCB-CR SLIP and its corresponding tectonic setting. Furthermore, the links between theSCB-CR SLIP and large-scale epithermal mineralization are discussed in details.

2. Geological Background and Rock Characteristics

The SCB comprises the Yangtze and Cathaysia blocks, and the two blocks are separated by the Jiang-ShaoFault (JSF). The two blocks were amalgamated together in the Neoproterozoic Jiangnan Orogeny alongthe JSF fault [Wang et al., 2012; Zheng et al., 2008]. The JSF fault, as a suture zone, later reactivated asa precursor to the development of the Nanhua rift basin [Wang and Li, 2003]. The Early PaleozoicKwangsian (Wuyi-Yunkai) Orogeny is characterized by the angular unconformity between pre-Devoniandeformed rocks and Devonian strata resulting from the northward underthrusting of the CathaysiaBlock beneath the Yangtze Block [Charvet et al., 2010; Ting, 1929]. The SCB experienced the TriassicIndochina Orogeny in response to the collision between the Indochina and South China blocks [Carteret al., 2001] and between the South China and North China blocks [Li et al., 2001; Ratschbacher et al.,2000]. Most researchers agree that the subduction of the paleo-Pacific plate beneath the South ChinaBlock occurred during the Yanshanian period (200 to 65Ma), although disagreement exists on in termsof the details of the subduction process [Gilder et al., 1996; Jiang et al., 2015; Li and Li, 2007; Sun et al.,2007; G. G. Wang et al., 2015a; Zhou et al., 2006].

The study area is located in the western region of Zhejiang province in the Cathaysia Block. The regional base-ment includes the Badu Group (or Badu Complex), which consists of sillimanite-mica schists, amphibolites,and gneisses, and represents the oldest rocks known in the Cathaysia Block [Yu et al., 2012]. Zircon U-Pb dat-ing and Lu-Hf isotopic analysis of the Badu complex, coeval granitoids, and intraplate basaltic rocks suggestthat two major episodes of crustal growth occurred in this region at 1.8–1.9 Ga and 2.7–2.9 Ga [Li, 1997; Yuet al., 2012; Zhao et al., 2014]. The cover lithologies are Yanshanian (200 to 65Ma) felsic volcanic rocks, whichcan be further divided into lower and upper volcanic series [Gu, 2005]. The lower volcanic series, i.e., theMoshishan Group, are subdivided into the Dashuang, Gaowu, Xishantou, Chawan, and Jiuliping formations.The lower volcanic series are widespread with a total outcrop area of more than 40,000 km2 and exhibit closespatial and genetic relationships with Au-Ag polymetallic deposits such as the Zhilingtou, Babaoshan, Wubu,and Dalingkou deposits [Pirajno et al., 1997].The upper volcanic series, i.e., Yongkang Group, are scattered indozens of basins and can be subdivided into the Guantou, Chaochuan, and Fangyan formations [The Bureauof Geology and Mineral Resources of Zhejiang Province, 1989].

The studied rock samples were collected from the Zhilingtou Au-Ag polymetallic deposit, which has24.5metric ton of Au at an average grade of 12.94 g/t and 527.7 t of Ag at an average grade of 278 g/t. Therock units in the Zhilingtou deposit include basement rocks of the Badu Group and cover rocks of theMoshishan Group (the lower volcanic series) (Figure 1b). The lower part of the Moshishan Group containsmedium-coarse grained quartz sandstones and tuffaceous sandstones with rhyolitic tuff interlayers at thebase and rhyolitic tuff breccia at the top. The upper part of the Moshishan Group simply contains a daciticvolcanic succession. In addition to volcanics, at least two stages of Late Mesozoic intrusive rocks occur inthe Zhilingtou deposit. A felsophyre occurs sporadically in the basement units of the Badu Group, and thecrosscutting relationships between volcanics and felsophyre are unclear. Bimodal intrusive rocks includingfelsite and diabase dykes intruded felsic volcanics of the Moshishan Group. The felsophyres are composedof K-feldspar, quartz, plagioclase, and biotite (Figures 2a and 2b). The rhyolites exhibit porphyritic texturesand consist mainly of quartz, alkaline feldspar, plagioclase, and biotite (Figures 2c and 2d). The dacites displaya porphyritic texture and contain plagioclase, quartz, alkaline feldspar, biotite, and hornblende (Figures 2eand 2f). The felsic member of the bimodal rocks is mainly composed of quartz, alkaline feldspar, and plagio-clase with minor amounts of biotite, whereas the mafic member is composed of biotite, plagioclase, hornble-nde, K-feldspar, and quartz (Figures 2g–2j).

3. Sampling and Analytical Methods

Zircons for cathodoluminescence (CL) imaging, U-Pb dating, and Lu-Hf isotopic studies were collectedfrom eight samples of the Zhilingtou volcanic and intrusive rocks. Thirty-six samples were chosen for



the analysis of the whole-rock major and trace elements, and nine samples were selected for the analysisof the Rb-Sr and Sm-Nd isotopes. A summary of the Zhilingtou igneous rocks is presented in Table 1. Thesupporting information provides data tables listing the zircon U-Pb isotope (Table S1), major and traceelement (Table S2), Sr and Nd isotope (Table S3), and zircon Hf isotope results (Table S4).

The zircon grains for LA-ICP-MS U-Pb dating were separated from the selected igneous rocks using con-ventional heavy liquid and magnetic separation methods. Representative zircon grains were handpickedunder a binocular microscope, mounted on an epoxy resin disk and polished down to nearly half the sec-tion to expose internal structures for LA-ICP-MS analysis. Zircons were documented with transmitted andreflected light photomicrographs and CL images to reveal their internal structures. The mounts werevacuum coated with high-purity gold prior to examination to avoid charging. The CL images were takenwith the scanning electron microscope at the State Key Laboratory of Continental Dynamics at NorthwestUniversity, and in situ LA-ICP-MS zircon U-Pb dating was performed using an Agilent 7500 ICP-MS,coupled with a 213 nm New Wave laser microprobe at the State Key Laboratory for Mineral DepositResearch at Nanjing University. Analytical procedures are described by Jackson et al. [2004]. CommonPb was corrected according to the method proposed by Andersen [2002]. The analyses presented herehave been corrected assuming recent lead loss. Data processing was carried out using Isoplot programsof Ludwig [2001].

Samples for elemental and Sr-Nd isotopic analysis were initially examined by optical microscopy to selectunaltered or the least altered samples. Major element contents of the samples were determined at theState Key Laboratory for Mineral Deposit Research at Nanjing University using an X-ray fluorescence spectro-meter, with a precision of better than 5%. Trace elements, including rare earth elements (REEs), were analyzedusing a Finnigan Element II ICP-MS at the State Key Laboratory for Mineral Deposit Research at NanjingUniversity following procedures described by Gao et al., [2003]. The analytic precision for trace and rare earthelements is better than 10%.

Sr and Nd isotopic compositions were measured using a Triton Thermal Ionization Mass Spectrometer at theState Key Laboratory for Mineral Deposit Research at Nanjing University, following the methods of by Pu et al.[2005]. 87Sr/86Sr and 143Nd/144Nd ratios are normalized to a 86Sr/88Sr value of 0.1194 for Sr and to a 146Nd/144Nd value of 0.7219 for Nd. During the analysis, measurements resulted in a 143Nd/144Nd ratio of0.511842� 4 (2σ, n= 5) for the La Jolla standard (recommended value = 0.511850) and 87Sr/86Sr ratio of0.710260� 10 (2σ, n= 30) for the NBS-987 Sr standard (recommended value = 0.710245). Total analyticalblanks were 5 × 10�11 g for Sm and Nd and 2 to 5 × 10�10 g for Rb and Sr.

The zircon Hf isotopic analysis was conducted in situ using a New Wave UP213 laser ablation microprobe,attached to a Neptune multicollector ICP-MS at the Institute of Mineral Resources at Chinese Academy ofGeological Sciences in Beijing. Instrumental conditions and data acquisition were comprehensively describedby Hou et al., [2007] and Wu et al., [2006]. A stationary spot was used for the present analysis, with a beamdiameter of 40 or 55μm depending on the size of ablated domains. The zircon GJ1 was used as a referencestandard during our routine analysis, with a weighted mean 176Hf/177Hf ratio of 0.281998� 0.000024 (2σ,n= 14). This value is undistinguishable from a weighted mean 176Hf/177Hf ratios of 0.282000� 0.000005(2σ) using the solution analysis method described by Morel et al. [2008]. Initial 176Hf/177Hf ratios εHf(t) werecalculated with the reference to the Chondritic Uniform Reservoir (CHUR) at the time of zircon growth fromthe magma. The adopted decay constant for 176Lu is 1.865 × 10�11 yr�1 [Scherer et al., 2001], and thechondritic176Hf/177Hf ratio of 0.282772 and 176Lu/177Hf ratio of 0.0332 are from Blichert-Toft and Albarède,[1997]. Two-stage model ages (TDM2) were calculated assuming 176Lu/177Hf = 0.015 for the average continen-tal crust [Griffin et al., 2002].

4. Results4.1. Zircon Petrography and U-Pb Dating

CL images of the representative zircon grains with 206Pb/238U ages and εHf(t) values are shown in Figure 3.Zircons are generally euhedral, prismatic (ranging from short to long), colorless, and transparent. The crystalgrains range from 60 to 240μm in length, with axial (length/width) ratios varying from 1:1 to 3:1. Most of the



zircons show oscillatory or planar zoning in the CL images (Figure 3), similar to zircons observed in typicallymagmatic rocks [Hoskin and Schaltegger, 2003].

LA-ICP-MS zircon U-Pb results of igneous rock samples are summarized in Tables 1, S1, and Figure 3. Weidentify four stages of magmatism at Zhilingtou. Thirty-two results from stage 1 felsophyre dikes are closeto the concordia curve and yield a weighted mean 206Pb/238U age of 149� 1Ma (n= 32, mean square [sumof] weighted deviation (MSWD) = 0.63). Twenty-eight analytical spots from stage 2 rhyolites have aweighted mean 206Pb/238U age of 128� 1Ma (n = 28, MSWD=1.01). Twenty-five spots from stage 3 dacitewere concentrated on a concordant curve and show a weighted mean 206Pb/238U age of 111� 1Ma(n= 25, MSWD=0.26). Bimodal rocks formed in stage 4 have a weighted mean 206Pb/238U age of101� 1Ma (n= 8, MSWD=0.06) and a weighted mean 206Pb/238U age of 100� 2Ma (n=13, MSWD=2.7)for diabase and felsite, respectively.

Figure 3. Typical CL images and LA-ICP-MS U-Pb concordant curves for zircons from the Zhilingtou igneous rocks.



The presented zircon U-Pb dating results suggest that four stages of volcanic and intrusive rocks in theZhilingtou area formed during the Late Jurassic to Early Cretaceous (circa 149 to 100Ma). Volcanic rocksformed in stages 2 and 3 and erupted at circa 128Ma and 111Ma, respectively. Intrusive rocks formed instages 1 and 4 and intruded at circa 149 and 100Ma, respectively.

4.2. Whole-Rock Elements

The whole-rock major and trace element data are presented in Table S2 and Figure 4, with 4 samples fromstage 1 felsophyre, 11 samples from stage 2 rhyolite, 9 samples from stage 3 dacite, and 5 and 7 samples fromstage 4 diabase and felsite, respectively.

Samples of stage 1 felsophyre have very high concentrations of SiO2 (77.09 to 77.34wt %), K2O (5.60 to6.02wt %), Rb (226 to 302 ppm), and high field strength elements (HFSEs, e.g., Zr, with values of 183 to

Figure 4. (a) TAS diagram [after Middlemost, 1994], (b) SiO2 versus Zr/TiO2 classification diagram after [Winchester andFloyd, 1977], (c) K2O versus SiO2 [after Le Maitre et al., 1989], (d) Mg# versus SiO2, data sources: G. G. Wang et al. [2014]and the references therein, (e) Sr/Y versus Y [after Defant et al., 2002], (f) P2O5 versus SiO2, and (g and h) Nb versus10,000*Ga/Al and Rb/Ba versus Zr + Ce + Y [after Whalen et al., 1987] for the igneous rocks at Zhilingtou.



Figure 5. Normalized REE patterns and trace element spidergrams for the volcanic-intrusive rocks in the Zhilingtoudeposit. Chondrite and primitive mantle data are from Boynton [1984] and Sun and McDonough [1989], respectively.Average OIB, OAB, and CAB data are from Sun and McDonough [1989] and Kelemen et al. [2003]. Abbreviations: OIB oceanicisland basalt, OAB oceanic arc basalt, and CAB continental arc basalt.



212 ppm), but low contents of TiO2 (0.12 to 0.13wt %), P2O5 (0.01 to 0.02wt %), Ba (46 to 74 ppm), Sr (17 to31 ppm), and Eu (0.05 to 0.13 ppm) (Tables 1 and S2). These samples plot in the region of granites on the TASdiagram (Figure 4a). They display obvious enrichment in light rare earth elements (LREEs) and marked Eudepletions in the REE patterns (Figure 5a). In spidergrams, they show negative Ba, Nb, Sr, Eu, and Ti anomaliesand positive Pb anomalies (Figure 5b). Elemental data suggest that stage 1 felsophyre can be classified as ahighly fractionated I-type granites [Wu et al., 2003] (Figures 4e and 4f).

Samples of stage 2 rhyolite have high SiO2 (67.92 to 76.11wt %), K2O (4.04 to 6.22wt %), and Rb (111 to331 ppm) contents but low MgO (0.20 to 1.43wt %) and Al2O3 (mostly less than 12.71wt %), Sr (11 to140 ppm) contents, low Mg# (25 to 37) values, and low Sr/Y (0.47 to 12.27) ratios (Tables 1 and S2). They plotin the domains of rhyolite and rhyodacite in the SiO2 versus Zr/TiO2*0.0001 diagram and belong to the high-Kcalc-alkaline series (Figures 4b and 4c). All the samples fall into the low Mg# region (Figure 4d). REE patternsexhibit a certain degree of LREE enrichment and negative Eu anomalies (Figure 5c). The spidergrams showthat they have typical arc magma geochemical affinities, such as clear enrichments in large ion lithophile ele-ments (LILEs) and Pb, but relative depletions of Nb, Ta, and Ti (Figure 5d) [Rudnick and Gao, 2003].

Sample of stage 3 dacite shows intermediate contents of SiO2 (64.46 to 70.20wt %), Al2O3 (13.92 to 16.28wt%), and Sr (237 to 473 ppm), high contents of K2O (3.00 to 5.78wt %), but low contents of MgO (0.42 to1.05wt %), low Mg# (28 to 35) values, and low Sr/Y (9.84 to 18.91) ratios (Tables 1 and S2). They fall intothe dacite domain in the SiO2 versus Zr/TiO2*0.0001 diagram and belong to the high-K calc-alkaline toshoshonitic series (Figures 4b and 4c). REE patterns exhibit a certain degree of LREE enrichment with noobvious Eu anomalies (Figure 5e). Similar to stage 2 volcanics, stage 3 volcanic rocks also show low Mg#values (Figure 4d), and an arc magma geochemical signature (e.g., Nb, Ta, and Ti depletions but Pb enrich-ment) (Figure 5f). However, unlike stage 2 volcanics, stage 3 volcanic rocks have higher P2O5, Sr, and Ba con-tents but lower SiO2 and Rb contents (Table S2 and Figure 4e).

Samples from stage 4 diabase have low SiO2 abundances of 44.91 to 47.11wt % and plot in the basalt regionin the SiO2 versus Zr/TiO2*0.0001 diagram and in the monzodiorite domain in the TAS diagram (Figures 4aand 4b). They have high contents of K2O (2.63 to 3.12wt %), Na2O (3.14 to 3.43wt %), MgO (4.37 to5.59wt %), Ba (477 to 2182 ppm), and Sr (586 to 2476 ppm) and high Mg# (44 to 55) values, but low contentsof Nb (13.5 to 15.5 ppm), Ta (0.75 to 0.89 ppm), and Ti (8163 to 9077 ppm) (Figures 4c and 4e and Tables 1 andS2). REE and trace element diagrams show that these samples are enriched in LREEs, LILEs (e.g., Ba and Sr),and Pb but depleted in Nb, Ta, and Ti (Figures 5g and 5h), suggesting a subduction-related metasomatizedmagma source [Sun and McDonough, 1989].

Samples from stage 4 felsite have high abundances of SiO2 (74.98 to 76.87wt %) and K2O (3.96 5.68wt %) butlow abundances of CaO (0.24 to 1.20wt %), MgO (0.09 to 0.26wt %), P2O5 (<0.01wt %), Nb (11.3 to 13.8 ppm),Ti (527 to 686 ppm), Sr (82 to 157 ppm), and Ba (434 to 605 ppm) as well as Mg values (16 to 36) (Tables 1 andS2). They plot in the granite domain in the TAS diagram and belong to the high-K calc-alkaline series(Figures 4a and 4c). They show enrichment in LREEs and a certain degree of negative Eu anomalies(Figure 5i). Compared with stage 1 felsophyre, stage 4 felsite lacks strong Eu, Sr, and Ba depletions, indicatinga relatively low degree of magma fractionation (Figures 4e and 4f). These samples show negative anomaliesin Ba, Nb, Sr, and Ti and positive anomalies in Pb in spidergrams (Figure 5j), suggesting a subduction-relatedmetasomatized magma source.

4.3. Whole-Rock Sr-Nd Isotopes

Whole-rock Rb-Sr and Sm-Nd isotopic compositions were determined for nine samples. These measured dataand calculated initial 87Sr/86Sr and 144Nd/143Nd ratios are presented in Tables 1 and S3 and Figure 6. The sam-ple from stage 1 felsophyre has low initial 87Sr/86Sr ratios of 0.703 in good agreement with its extremely highRb/Sr ratio of 13.5. Stage 1 felsophyre has a εNd(t=149Ma) value of �5.2 and a two-stage Nd model age(TDM2) of 1.36 Ga (Table S3). Rhyolite and dacite samples from stages 2 and 3 have similar Sr-Nd isotopic com-positions, with initial 87Sr/86Sr ratios of 0.711 to 0.714, negative εNd(t= 128–111Ma) values of �7.6 to �5.8,and two-stage Nd model ages (TDM2) of 1.38 to 1.53Ga (Table S3 and Figure 6). Compared with stages 2and 3 rocks, the bimodal rock samples from stage 4 have similar initial 87Sr/86Sr ratios of 0.707 to 0.712 buthigher εNd(t= 111–100Ma) values of �5.0 to +0.2 and lower two-stage Nd model ages (TDM2) of 0.89 to1.31Ga (Table S3 and Figure 6).



4.4. Zircon Hf Isotopes

Eight samples that were dated using thezircon U-Pb method were also analyzedby LA-MC-ICP MS to measure the Lu-Hfisotopes in the same domains or similarstructures. Initial 176Hf/177Hf ratiosdenoted by εHf(t) values and two-stageHf model ages for the analyzed zirconswere calculated using weighted meanage. The zircon Hf isotopic data are listedin Tables 1 and S4 and Figure 7.

Eighteen analyses for stage 1 felsophyreyield very negative εHf(t) values of �18.6to �14.0 (Figure 7a). They correspond totwo-stage Hf model ages (TDM2) rangingfrom 2.08 to 2.36 Ga (Table S4). Zircongrains from stage 2 rhyolite exhibit rela-tively higher negative εHf(t) values of�13.5 to �1.8 (Figure 7b).Correspondingly, their two-stage Hf modelages (TDM2) range from 1.30 to 2.02 Ga(Table S4). Twenty-three analyses for stage

3 dacite show Hf isotopic compositions similar to the analytical data for stage 2 rhyolite. Stage 3 dacite hasnegative εHf(t) values of �11.5 to �3.6 and two-stage Hf model ages (TDM2) ranging from 1.39 to 1.89Ga(Figure 7c and Table S4). Zircon grains from stage 4 bimodal rocks have slightly higher εHf(t) values, withεHf(t) values of �8.1 to �2.2 (Figure 7d). The corresponding two-stage Hf model ages (TDM2) range from1.30 to 1.67 Ga (Table S4).

Figure 6. εNd(t) versus (87Sr/86Sr)i diagram showing the isotopes for

the volcanic-intrusive rocks in the Zhilingtou deposit. Data for theDexing juvenile crust-derived felsic rocks are taken from G. G. Wanget al. [2015a]. Data for MORB and the approximate fields of mantlereservoirs are taken from Zindler and Hart [1986] and referencestherein. Data for the Darongshan S-type granite are taken from Qiet al. [2007].

Figure 7. Histograms of in situ zircon εHf(t) values of the volcanic-intrusive rocks in the Zhilingtou deposit.



5. Discussion5.1. Petrogenesis of the ZhilingtouVolcanic-Intrusive Complex5.1.1. Hf and Nd Isotopes asIndicators of Crustal Residence Timeand Their DecouplingThe variations in Hf and Nd isotopiccompositions have been well developedas an unambiguous petrogenetic indica-tor to decipher the continental crustalgrowth and evolution because of radio-active decay of 147Sm and 176Lu[DePaolo et al., 1991; Harrison et al.,2005; Vervoort et al., 1996]. εHf(t) andεNd(t) values have generally been usedto indicate the deviation of the176Hf/177Hf and 143Nd/144Nd values ofthe sample from that of the CHUR inunits of parts in 104, respectively[DePaolo, 1988; Vervoort et al., 2000].Generally speaking, the Hf and Nd

isotopes of igneous rocks derived from recycled ancient continental crustal rocks with low Sm/Nd andLu/Hf ratios have negative εHf(t) and εNd(t) values, while those of igneous rocks derived from the depletedmantle with high Sm/Nd and Lu/Hf ratios have positive εHf(t) and εNd(t) values [Flierdt et al., 2002; Harrisonet al., 2005]. The depleted mantle model age (TDM) has been used to quantitatively constrain the crustalresidence time of magma source of depleted mantle-derived rocks that generally have positive εHf(t) andεNd(t) values [DePaolo et al., 1991]. In contrast, the two-stage model age (TDM2) assumes that the parentalmagma was produced from ancient continental crust that commonly has negative εHf(t) and εNd(t) values[Vervoort and Blichert-Toft, 1999]. Given that the Zhilingtou igneous rocks have negative εHf(t) and εNd(t)values (Tables 1, S3 and S4), we use the two-stage model age (TDM2) for zircon Hf and whole-rock Nd iso-topes to express the crustal residence time.

As summarized in Table 1, the two-stage whole-rock Ndmodel ages of the Zhilingtou volcanic-intrusive com-plex are clearly lower than the two-stage zircon Hf model ages (TDM2). Therefore, it is necessary to determinewhich isotope system is reliable before using them to discuss the magma source signature. The Nd isotopedisequilibrium is common between crustal protoliths and melts formed by crustal anatexis, because theREE budget (e.g., Nd) can be controlled by accessory phases (e.g., garnet, apatite, and monazite) [Ayres andHarris, 1997; Davies and Tommasini, 2000]. For example, the batch melting modeling implied that the proto-lith with a real model age of 1.7 Ga yielded melts with an unrealistic estimated Nd model ages ranging from0.66 to 2.24 Ga due to the Nd isotope disequilibrium [Davies and Tommasini, 2000]. In contrast, zircon Hf iso-topes are much more reliable because (1) zircon has high Hf concentrations and low Lu/Hf ratios; (2) the crys-tallization age can be directly dated by zircon U-Pb techniques; (3) zircon is extremely resistant to Lu/Hfdisturbance; and (4) it is easy to monitor whether the zircon Lu-Hf isotopic system is closed via the combineduse of the U-Pb system [Amelin et al., 1999; Kemp et al., 2006; Vervoort et al., 1996]. As a consequence, in thisstudy, we used zircon two-stage Hf model age (TDM2) in order to trace the magma source and origin ofigneous rocks.5.1.2. Petrogenesis of Stage 1 FelsophyreStage 1 felsophyre has very negative εHf(t) values of �18.6 to �14.0 and relatively old two-stage Hf modelages (TDM2) from 2.08 to 2.36 Ga, suggesting that it is primarily derived from ancient rather than juvenilecrust [G. G. Wang et al., 2014; Xiong et al., 2014]. Detrital zircons from the Oujiang River in the EastCathaysia Block indicate that the basement in Zhejiang province is dominantly Paleoproterozoic in age(1. 85 to 2.40Ga) with minor Archean components [Xu et al., 2007]. The zircon Hf isotopes from stage1 felsophyre plot in the area of crustal evolution of the East Cathaysia Block (Figure 8), indicating thatstage 1 felsophyre was likely generated by melting of Cathaysia Block continental crust. Together with

Figure 8. Diagram of εHf(t) versus U-Pb ages for zircons from theZhilingtou volcanic and intrusive rocks. The full line of crustal extractionis calculated by using 176Lu/177Hf ratio of 0.015 for the average conti-nental crust. The data for the basement in East Cathaysia are from XishengXu et al. [2007]. Symbols are the same as those in Figure 4.



the low MgO contents and Mg# values (Table 1) of the Zhilingtou stage 1 felsophyre, few mantle materi-als were involved in parental magmatic melt.

Stage 1 felsophyre has very high contents of SiO2, Rb, and HFSEs (e.g., Zr, Nb, Ce, and Y) but extremely lowcontents of P2O5, Eu, Ba, and Sr, indicating that it can be classified as a highly fractionated I-type granite(Table S1 and Figures 4 and 5). Essential minerals in stage 1 felsophyre are quartz, perthite, and plagioclasewith minor biotite, implying that magmas of stage 1 felsophyre experienced significant fractionation.Strong fractional crystallization is demonstrated by significant depletions in Ba, La, Ce, Sr, Eu, and Ti inthe spidergrams (Figures 5a and 5b). The obvious Eu, Sr, and Ba depletions likely result from extensivefractionation of plagioclase and K-feldspar, the strong Nb and Ti negative anomalies require Ti-bearingphase separation (e.g., ilmenite and titanite), and the clear P depletion is related to apatite separation

[G. G. Wang et al., 2014; Wu et al.,2003]. As shown by the Sr-Ba diagram(Figure 9a and Table S5), the stage 1 fel-sophyre data plot in the region amongthe plagioclase, K-feldspar, and biotiteevolutional lines. Because K-feldsparincreases during magma differentiation,K-feldspar is likely not the componentresponsible for the depletion of Sr andBa [Wu et al., 2003]. The reasonableexplanation is that the fractionation ofplagioclase occurred during the earlystage and the fractionation of plagio-clase and biotite developed during thelate stage. Additionally, the accessoryminerals appear to affect much of theREE variation. In the diagram of (La/Yb)Nversus La, the variation in REE contentsseems to be consistent with the separa-tion of monazite and allanite, apatite,and sphene but is not influenced by zir-con separation (Figure 9b and Table S6).5.1.3. Petrogenesis of Stages 2 and 3Felsic VolcanicsMafic microgranular enclaves (MMEs)occur in some Late Mesozoic igneousrocks in the SCB-CR [Li et al., 2014; Xuet al., 1999], and these igneous rocks com-monly have higher zircon εHf(t) andwhole-rock εNd(t) values than basementrocks in the Cathaysia Block [Guo et al.,2012; Li et al., 2014; Liu et al., 2015], indi-cating that a magma mixing processoccurred. However, the lack of MMEs inthe Zhilingtou felsic volcanics stronglyargues against magma mixing. Inaddition, the Zhilingtou felsic volcanicshave a low-Mg geochemical signature(Table 2 and Figure 4d), precluding thepossibility of a significant input ofmantle-derived mafic melts. Thus, magmamixing is unlikely to have generated theZhilingtou stages 2 and 3 felsic volcanics.

Figure 9. Modeling fractionation process during the generation ofstage 1 felsophyre in the Zhilingtou deposit. (a) Ba versus Sr diagramshowing the separation of plagioclase and biotite. Partition coefficientsof Sr and Ba are from Hanson [1978]. (b) (La/Yb)N versus La diagramshowing separation of accessory minerals, especially allanite, monazite,and apatite. Partition coefficients are from Arth [1976] for apatite, Greenand Pearson [1986] for titanite, Mahood and Hildreth [1983] for zircon,Green et al. [1989] for allanite, Yurimoto et al. [1990] for monazite, andWu et al. [2003] for hornblende. Abbreviations: Cpx = clinopyroxene,Opx = orthopyroxene, Hbl = hornblende, Bi = biotite, Pl = plagioclase,Kf = K-feldspar; Ap = apatite, Allan = allanite, Sph = sphene,Mon =monazite, Zr = zircon. The blue filled diamond symbols are thesame as those in Figure 4, and the red filled yellow square aresamples from the selected candidate representing parent magma[G. G. Wang et al., 2014]. Data for modeling fractional crystallization ofstage 1 felsophyre are listed in Tables S5 and S6. Modeling procedurefor fractional crystallization is described in Text S1.



The low-Mg geochemical signature strongly argues against the direct contribution of mantle materials intothese felsic volcanics, whereas juvenile continental crust is a good candidate to explain the higher εHf(t)values [Vervoort and Patchett, 1996; G. G. Wang et al., 2015a; Zheng et al., 2008]. Growth of the juvenile crustlikely occurred during the Early Cretaceous in the SCB-CR. First, most of Hf isotope data from stages 2 and 3felsic volcanics display systematically higher zircon εHf(t) values (�13.5 to �1.8) than those from stage 1 fel-sophyre (Table S2) and basement rocks in the Cathaysia Block [Xu et al., 2007]. As shown in the t-εHf(t) diagram(Figure 8), stages 2 and 3 felsic volcanic samples plot above the evolutionary trend of the basement rocks inthe Cathaysia Block. Second, the Early Cretaceous igneous rocks in the SCB-CR have the youngest Hf-Ndmodel ages and lowest initial Sr isotopes among those in South China, indicating that the input of the asth-enospheric mantle materials resulted in significant crustal growth [Gilder et al., 1996]. The newly underplatedjuvenile crustal materials during the Early Cretaceous beneath the SCB-CR could be gabbroic sills in composi-tions near the crust-mantle transition zone similar to those described in the Oman ophiolites [Kelemen et al.,1997]. This phenomenon is supported by the fact that mantle-derived mafic magmas are denser than mostcrustal rocks and therefore tend to pool near the base of the crust to form an underplated layer [Richards,2003]. Besides as part of magma source materials, the underplated basaltic magma likely also provides a sig-nificant amount of heat for crustal anatexis and the eruption of large-scale felsic volcanism [Wilkinson, 2013].Therefore, partial melting of the mixture of newly underplated juvenile and ancient continental crust materi-als likely explains the genesis of stages 2 and 3 low-Mg felsic volcanics.

Stages 2 and 3 volcanics show various major and trace element concentrations, which can be explained bysource differences or magmatic processes. They share similar εHf(t) values and two-stage Hf models ages, sug-gesting that they have similar magma sources and probably have constant proportions of juvenile andancient crustal materials. Thus, magmatic processes play a crucial role in the changes in the geochemicalcompositions of these felsic volcanics. The observed variations in the magma compositions can be generatedby different degrees of magma fractionation or partial melting. Figure 10 displays data from stage 2 and 3 onZr/Nb versus Zr and La/Sm versus La diagrams. In both diagrams, the data show increasing Zr/Nb and La/Smratios with increasing Zr and La content, respectively, revealing geochemical trends that are consistent withpartial melting rather than fractional crystallization. Hence, we conclude that partial melting is the predomi-nant process responsible for the formation of the Zhilingtou felsic volcanics.5.1.4. Petrogenesis of Stage 4 Bimodal RocksCompared to the Zhilingtou intermediate to acid rocks, stage 4 diabase has lower concentrations of SiO2

(44.91 to 47.11wt %) and higher MgO (4.37 to 5.59wt %), indicating that it is the most mafic rocks in theZhilingtou region. Stage 4 diabase has trace element patterns similar to those of OIBs, except for the deple-tions in Nb, Ta, and Ti. Additionally, the εNd(t) and εHf(t) values of the diabase are higher than those of theenriched mantle end-members (EMI or EMII, Figure 6). The high incompatible element contents and εNd(t)and εHf(t) values reveal that a significant contribution of the depleted asthenospheric mantle. In addition,stage 4 diabase has much lower εNd(t) and εHf(t) values than typical the depleted asthenospheric mantle, indi-cating strong metasomatism likely occurred in the mantle source region or crustal contamination took placethe ascent of mantle-derived magma to the shallow crustal environments. Stage 4 diabase has very high Sr

Figure 10. Partial melting discriminative diagrams for the Zhilingtou felsic volcanics. (a) Zr/Nb versus Zr diagram; (b) La/Smversus La diagram. Abbreviations: PM = partial melting; FC = fractionation crystallization. Symbols are the same as those inFigure 4.



contents and lacks a negative Ta anomaly, which is a contrast to the coeval crust-derived felsite, suggestingthat it experienced little crustal contamination. The enrichments in LILEs (Ba, Th, Pb, La, Ce, etc.) and deple-tions in the HFSEs (Nb, Ta, Ti, etc.) of stage 4 diabase are similar to average compositions of arc basalts(Figures 5g and 5h), suggesting that the mantle source region was metasomatized in an arc or back-arc set-ting. An arc or back-arc setting for stage 4 diabase is consistent with by the NW directed subduction of thepaleo-Pacific plate beneath the South China along its southeastern margin during Late Mesozoic [Sunet al., 2007; G. G. Wang et al., 2015a; Zhou et al., 2006]. The absence of a negative Eu anomaly in thechondrite-normalized REE patterns and the presence of a positive Sr anomaly in the spidergrams precludesignificant fractional crystallization of plagioclase, indicating that little magma fractionation occurred duringthe generation of stage 4 diabase.

Similar to stages 2 and 3 felsic volcanics, stage 4 felsite has higher εHf(t) values than basement rocks in theCathaysia Block (Figures 7 and 8), implying involvement of newly underplated juvenile crust or mantle mate-rials as magma sources. The extremely low Mg content of stage 4 felsite (Table 1) strongly argues against amantle source but supports a mixed source involving newly underplated juvenile crust and ancient continen-tal crust. Partial melting of the juvenile continental crust likely resulted from upwelling of coeval hot basalticmelts of metasomatized mantle. The high SiO2 contents of the stage 4 felsite commonly indicate a highdegree of fractionation. However, the weak Eu and Sr negative anomalies in the normalized REE patternsand spidergrams (Figures 5i and 5j) suggest no strong feldspar fractionation occurred. Thus, partial meltingand slight fractionation are likely responsible for the formation of stage 4 felsite.

5.2. Spatiotemporal Distribution of the SCB-CR SLIP

The formation ages of the SCB-CR SLIP have drawn great attention over the past few decades because of theirtectonic significance and their relation to large-scale epithermal mineralization. Geologists originally pro-posed that abundant volcanic successions in Zhejiang, Fujian, and Guangdong provinces mainly formed dur-ing the Middle to Late Jurassic, with minor episodes during the Cretaceous [The Bureau of Geology andMineral Resources of Fujian Province, 1985; The Bureau of Geology and Mineral Resources of ZhejiangProvince, 1989], based on various methods such as K-Ar, 40Ar-39Ar, Rb-Sr, and U-Pb methods on single miner-als or whole rocks [Li et al., 1989; L Liu et al., 2012; Yang et al., 2008; Yu and Xu, 1999]. However, the relativelylow closure temperatures do not preclude resetting of both K-Ar and Rb-Sr isotope systems associated withlater thermal disturbances [Dodson, 1973; Li et al., 1999]. In contrast, the U-Pb isotopic analysis on individualzircon is regarded as a reliable method due to higher closure temperatures [Cliff, 1985]. Recently, someJurassic to Cretaceous ages have been reported based on SHRIMP or LA-ICP-MS single grain zircon U-Pb ana-lysis of felsic volcanics from Guangdong and Fujian provinces [Guo et al., 2012; Liu et al., 2015]. In addition,felsic volcanics from northern and southeastern Zhejiang province are dated to yield a Cretaceous formationage (circa 140 to 88Ma) [L. Liu et al., 2012a]. The dating results of the Zhilingtou rhyolites and dacites suggestthat voluminous felsic volcanics of the Shimaoshan Group in southwestern Zhejiang province formed duringEarly Cretaceous (circa 128 to 110Ma). Therefore, our results provide a robust age constraint on voluminousfelsic volcanics throughout Zhejiang province and suggest that the formation ages are Early Cretaceous toearly Late Cretaceous instead of the previously proposed Middle to Late Jurassic formation ages.

The data on volcanics in southwestern Zhejiang (e.g., the Zhilingtou volcanics), together with recentlyobtained data on volcanics from northern and southeastern Zhejiang, Guangdong, and Fujian provinces[Guo et al., 2012; L. Liu et al., 2012a, 2015], provide a great opportunity to reconstruct the spatiotemporal fra-mework of the entire SCB-CR SLIP. In the following we provide a summary of the three episodes of volcanismthat occurred in the SCB-CR. The first volcanic sequence formed during the Middle to Late Jurassic and ischaracterized by minor occurrences of felsic volcanic rocks in northeastern Guangdong and southernFujian provinces (168–145Ma) [Guo et al., 2012] as well as minor dacite and felsophyre in southeasternZhejiang province (177Ma) [L. Liu et al., 2012a; this study]. The second Early Cretaceous felsic volcanic succes-sion is predominant and constitutes the main part of the SCB-CR SLIP in Zhejiang and northern Fujian pro-vinces (143–110Ma) [Guo et al., 2012; L. Liu et al., 2012a, 2015; this study]. The third episode of LateCretaceous bimodal volcanic-intrusive rocks occur along the easternmost coastline in the SCB-CR, and ourdating results suggest that they formed during 110 to 90Ma [Liu et al., 2015; this study]. The new spatiotem-poral framework is characterized by minor Middle to Late Jurassic felsic volcanic rocks in northeasternGuangdong and southern Fujian provinces, voluminous Early Cretaceous volcanics in Zhejiang and northern



Fujian provinces, and minor Late Cretaceous bimodal volcanic-intrusive rocks along the easternmost coast-line of SCB. The newly established spatiotemporal framework of the SCB-CR SLIP demonstrates a northwest-ward migration of the volcanic activity during 170 to 110Ma followed by an eastward migration during 110to 90Ma.

5.3. Tectonic Evolution of the SCB-CR SLIP

Althoughmost current studies support a subduction model of the paleo-Pacific plate along the margin of theSouth China Block during Late Mesozoic [Jiang et al., 2015; Li and Li, 2007; Q. Liu et al., 2012b; Sun et al., 2007;Zhou et al., 2006], two key issues including the subduction initiation time and the principal drifting directionof the subducting plate remain controversial. The subduction of the paleo-Pacific plate has been suggestedby some authors to have started in the Late Permian (circa 250Ma) [Li and Li, 2007] or Early Jurassic (circa197Ma) [Jiang et al., 2015]. However, the South China Block is characterized by ~ E-W tectonic elements inthe Triassic and Early Jurassic [Zhang et al., 2009] and this orientation is inconsistent with the coeval westwardsubduction of the paleo-Pacific plate. Additionally, the voluminous felsic arc volcanics in the SCB-CR SLIPwere produced during the Middle Jurassic to Early Cretaceous (Figure 11) rather than the Late Permian orEarly Jurassic. Furthermore, the absence of the contemporaneous accretionary wedge along the margin ofthe South China Block strongly argues against the Late Permian or Early Jurassic initial subduction. The initia-tion of the paleo-Pacific plate subducting beneath the South China Block most likely occurred in the MiddleJurassic [Dong et al., 2008; Isozaki, 1997; G. G. Wang et al., 2015a; Y. Wang et al., 2015b; Zhou et al., 2006]. Thisinterpretation is supported by the following observations: (1) the initial rapid formation of the Pacific plate at

Figure 11. Distribution of three episodes of volcanic successions in the SCB-CR SLIP. ZJ = Zhejiang, FJ = Fujian,GD = Guangdong, JX = Jiangxi, and HN=Hunan. The age data are from Guo et al. [2012], L. Liu et al. [2012, 2015], Wanget al., [2012], and this study.



circa 175Ma in response to the rapid breakup of the Pangean supercontinent (Figure 12a) [Storey, 1995;Veevers, 2004]; (2) the widespread development of Jurassic accretionary complexes along the East Asian con-tinental margin such as the Mino-Tanba and Chichibu belts in Southwest Japan, the Helongjiang Complex inNE China, the Tananao Complex in Taiwan, and the North Palawan Block in the west Philippines [Isozaki, 1997;Fu-Yuan Wu et al., 2007; Yui et al., 2012]; (3) the change from nearly E-W trending folding during the Triassic toEarly Jurassic to NNE trending faulting and folding during the Middle Jurassic in South China and nearbyregion [Y. Wang et al., 2015b; Zhang et al., 2009]; and (4) the marine regression in the Yongmei Basin inFujian province during approximately the late Early Jurassic and the initiation of felsic continental volcanismduring the Middle Jurassic [Xing et al., 2002].

The main drifting direction of the subducting paleo-Pacific plate is another crucial issue, and at least two dif-ferent viewpoints have been proposed [Goldfarb et al., 2007; Li and Li, 2007;Q. Liu et al., 2012b; Sun et al., 2007;Wang et al., 2011]. The Pacific plate drifted southwestward during 180–125Ma according to Wang et al.[2011]. This model plausibly explains systematical distribution of the Late Mesozoic large-scale igneousevents and associated mineralization in South China from NE to SW [Wang et al., 2011; Zhang et al., 2013].However, the spatiotemporal framework of the SCB-CR SLIP indicates that the felsic arc volcanism experi-enced an obvious northwestward shift during the Jurassic to Early Cretaceous (Figure 11), which stronglyargues against the existence of coeval southwestward subduction. In addition, porphyry-skarn Cu-(Au)deposits including the Dexing, Yinshan, Yongping, Dongxiang, Jiande, Baoshan, Qibaoshan, and

Figure 12. Tectonic evolution history of the SCB-CR SLIP in South China. (a and b) Plate reconstruction at 160Ma andnarrow arc magmatism in the SCB-CR between circa 170 and 140Ma; (c and d) plate reconstruction at 120Ma and widearc magmatism in the SCB-CR 140 to 110Ma; (e and f) plate reconstruction at 100Ma and bark-arc magmatism in theSCB-CR 110 to 90Ma. Plate reconstruction at 160Ma, 120Ma, and 100Ma is after Wessel and Müller [2015]. La = Laurasia;SA = South America; NA = North America, SCB = South China Block, MT =Meso-Tethys, WG =Western Gondwanaland;EG = Eastern Gondwanaland, Ch = China, Pac = Pacific, Phx = Phoenix, Far = Farallon, Iza = Izanagi.



Yuanzhuding deposits are primarily distributed along the NE trending Jiang-Shao Fault and have similarmetallogenic ages ranging from Middle to Late Jurassic [Li et al., 2015; Mao et al., 2011; Wang et al., 2013].More importantly, the Pacific plate first formed at circa 175Ma and was merely a small triangular plate farfrom South China until 140Ma (Figure 12a) [Bartolini and Larson, 2001; Müller et al., 2008]. As a consequence,the southwestward drifting history of the Pacific plate before circa 125Ma [Sun et al., 2007] should not be sim-ply used to discuss the Late Mesozoic setting of South China. The subducting plate beneath the South ChinaBlock from the Middle Jurassic to Early Cretaceous is most likely the Izanagi plate [Engebretson et al., 1985;Müller et al., 2008; Whittaker et al., 2007], which moved NWward or NNWward (Figures 12a, 12c, and 12e)[Goldfarb et al., 2007; Seton et al., 2012] and controlled the SCB-CR SLIP.

Because previous tectonic models cannot interpret well the spatiotemporal framework of the SCB-CR SLIP,the subduction initiation time, and the principal drifting direction of the subducting plate, it is necessaryto propose a new three-episode tectonic model. Episode 1 (circa 170 to 140Ma): minor arc volcanics formedlocally along the Zhenghe-Dapu Fault in Fujian and Guangdong provinces, suggesting that the initial north-westward subduction of the Izanagi plate beneath the South China Block [Gilder et al., 1996] likely occurred inthe Middle Jurassic and that a narrow volcanic arc formed (Figures 12a and 12b). Episode 2 (circa 140 to110Ma): the widespread felsic volcanic succession in Zhejiang and northern Fujian provinces suggests thatnorthwestward gradual subduction occurred and that a broad subduction zone formed during the EarlyCretaceous. In general, the width of the subduction zone is related to the slab dip [Gutscher et al., 2000;Tatsumi, 2005], and thus, the broad subduction zone in South China likely resulted from the shallow slab sub-duction of the Izanagi plate at that time (Figures 12c and 12d). Episode 3 (circa 110 to 90Ma): the LateCretaceous magmatism was characterized by prevailing bimodal volcanic-intrusive rocks along the eastern-most part of the SCB-CR, suggesting a back-arc setting. We propose that the opening of the Shi-Hang back-arc basin system [Gilder et al., 1996] resulted from the eastward retreat of the trench system due to roll back ofthe subducting Izanagi plate (Figures 12e and 12f).

5.4. Implication for Epithermal Mineralization in the SCB-CR SLIP

The SCB-CR SLIP is characterized by large-scale epithermal mineralization, including the Zhilingtou (24.5metricton Au and 528metric ton Ag), Wubu (645metric ton Ag), Dalingkou (870metric ton Ag), Dongyang (10metricton Au), Zijinshan (313metric ton Au), and Yueyang (1843metric ton Ag) deposits [The No. 7 Team of theZhejiang Bureau of Geology and Mineral Resources, 2006; Pan et al., 2015; Zhang et al., 2012]. With regards tothe large-scale epithermal mineralization in subduction zone (e.g., Zhilingtou), it remains a conundrumwhetherthe metal is derived from the mantle or the overriding continental crust [Chiaradia, 2014; Lee et al., 2012;Mungall, 2002;Wilkinson, 2013]. One view is that melting of themantle wedge destabilizes sulfides and releasesthe metals into the melt, forming the metal-rich magma [Ling et al., 2009; Mungall, 2002]. This hypothesisrequires that the ore-related magmas show significant contribution of mantle materials; thus, they are charac-terized by highMgO contents andMg values [Stern and Kilian, 1996]. However, the lowMg, Cr, and Ni geochem-ical characteristics of the Zhilingtou arc volcanics argue against the involvement of mantle-derived magmas(Table 1 and Figure 13a). An alternative view is that melting of the continental curst can form ore deposits with-out the contribution from the mantle [Chiaradia, 2014; Lee et al., 2012]. Our results suggest the Zhilingtou ore-related volcanics, probablymost of felsic volcanics in the SCB-CR, formed by remelting of the newly underplatedjuvenile basic continental crust, indicating the significant contribution of the continental crust rather than themantle. The newly underplated juvenile crustal materials could have formed beneath the SCB-CR during theEarly Cretaceous resulting from mantle-derived basaltic melts stalling near the crust-mantle transition zonedue to the relatively high density of basaltic magma [Kelemen et al., 1997].

Continental crust is generally thought to have lower metal concentrations than primary basaltic magmas inarc environments [Mungall, 2002; Wang et al., 2006]. However, juvenile continental crust may not adhere tothis pattern. In fact, the metal released from the subduction-modified mantle can be transported to the baseof the crust by mantle-derivedmafic magma, resulting in an initial enrichment. Such an initial enrichment hasbeen observed in natural environment, for example, high concentrations of Au are present in subarc mantlexenoliths near Lihir Island, Papua New Guinea [McInnes et al., 1999]. Additionally, the importance of this typeof initial metal enrichment in juvenile crust for ore deposits has also been advocated by many authors, basedon the Pb isotope constraints, the precise dating of ancient mineralization, and the geochemistry of ore-related porphyries [Core et al., 2006; Lee et al., 2012; Q. Liu et al., 2012b; Pettke et al., 2010; Richards, 2013;



Sillitoe et al., 2014; G.G. Wang et al., 2015a]. Thus, remelting of the metal-enriched juvenile lower continentalcrust may be a necessary step for the formation of a large number of epithermal deposits, particularly for low-Mg felsic volcanics in subduction zones.

Crustal thickness likely plays an important role in controlling the occurrence of the large-scale mineralizationin the subduction zone [Haschke et al., 2006; Kay et al., 1999]. Rare earth elements (REE) fractionation (e.g.,LaN/YbN ratios) provides useful information to predict the crustal thicknesses via pressure-sensitive residualminerals [Kay and Mahlburg-Kay, 1991]. The LaN/YbN ratios reflect pressure-dependent changes from clino-pyroxene to amphibole to garnet in the residual mineralogy in the magma source region. Low ratios ofLaN/YbN (≤20) generally indicate clinopyroxene-dominated mineral residues (30–35 km depth), intermediateratios (LaN/YbN> 20–30) indicate amphibole-dominated mineral residues (40 km depth), and high ratios(LaN/YbN≥ 30) reflect garnet-bearing mineral residues [Kay and Mahlburg-Kay, 1991; Rapp and Watson,1995]. In Figure 13b, the Zhilingtou felsic volcanics have low LaN/YbN ratios (9.93 to 19.45) suggesting a thincontinental crust (30–35 km depth). In contrast, the Middle Jurassic Dexing porphyry deposits have higherLaN/YbN ratios (up to 33.16), indicating a thickened crust (≥40 km depth). Similarly, the central Andean por-phyry Cu mineralization (e.g., EI Teniente and EI Indio)-related porphyries also have high LaN/YbN ratios(up to 36.1), which are attributed to crustal thickening induced by the repeated Chilean type flat-slab subduc-tion [Kay et al., 1999]. The comparison between epithermal and porphyry mineralization-related igneousrocks indicates low LaN/YbN ratios and thin continental crust favored the formation of SLIPs and relatedlarge-scale epithermal mineralization such as the Zhilingtou deposit (Figure 13c). In contrast, the porphyrymineralization should be generated in a thickened crust setting such as the Dexing ore field (Figure 13d).

The Pb element is mobile in the subduction zone environment, and its contents increase significantly whenslab subduction begins. The low Pb contents at circa 148Ma (Figure 14a) suggests that the Zhilingtou regionwas an intraplate setting at that time and the presence of a narrow arc in the SCB-CR during the Jurassic. ThePb concentrations are higher in the Zhilingtou igneous rocks formed after circa 128 (Figure 14a), indicatingthat a broad arc occurred during Early Cretaceous. The Pb concentrations are higher in the Zhilingtou igneousrocks formed after circa 110Ma (Figure 14a), suggesting that a slab rollback-related back-arc setting occurredduring the Late Cretaceous (after circa 110Ma). Such changes are also supported by the variations in the

Figure 13. (a) MgO versus SiO2 diagram for the igneous rocks in the Zhilingtou deposit: Data are sourced from G. G. Wanget al.[2015a] and reference therein; (b) LaN/YbN versus YbN for the igneous rocks in the Zhilingtou deposit [afterDrummondand Defant, 1990]; (c) epithermal deposits in the SCB-CR SLIP (e.g., Zhilingtou) formed by remelting of metal-rich nearlyunderplated juvenile crust in an arc setting; (d) porphyry deposits in the SCB (e.g., Dexing) formedbymelting of delaminatedsubcontinental lithospheric mantle and thickened continental crust.



mean zircon εHf(t) values (Figure 14b) and the variations in the distancebetween trench and arc volcanics(Figure 14c). The Zhilingtou Au-Agdeposit developed at circa 110Ma(this study) and the giant Zijinshanepithermal Au-Cu ore depositformed at circa 111Ma [Jiang et al.,2013]. Ages of host rocks at theZhilingtou and Zijinshan depositssuggest that the large-scale epither-mal mineralization was probablyproduced in a specific environmentin response to the transition from acontinental arc setting to a back-arcsetting (Figures 14c and 14d). Thecontinental arc setting (circa 140 to110Ma) commonly represents acompressional environment, butthe back-arc setting indicates anextensional regime (after circa110Ma). During the transitional fromarc to back-arc settings, the relaxa-tion of stress commonly reactivatepreexisting faults, which providechannels favorable to ore fluidsascent, resulting in precipitationand ore deposit formation in theshallow crust. The coupling betweenchanges in crustal stress regime and

the generation of epithermal deposits was also identified in Bajo de la Alumbrera in Argentina, Bingham inUSA, and Ok Tedi and Ertsberg in Papua New Guinea [Sillitoe, 2008; Solomon, 1990]. Similarly, we concludethat the tectonic transition from arc to back-arc settings in the SCB-CR provides a favorable environment thatexplains the development of the large-scale epithermal mineralization associated with theSLIP emplacement.

In summary, the large-scale epithermal mineralization in the SCB-CR SLIP is associated with melting of themetal-rich juvenile continental crust rather than the mantle. In addition, the Early Cretaceous epithermalmineralization in the SCB-CR SLIP is related to a thin arc resulting from the tectonic transition from arc toback-arc regimes. In contrast, the Jurassic porphyry mineralization in the South China Block correlates tothe thickened continental crust in an intraplate environment. Thus, we concluded that the large-scaleepithermal mineralization was generated by melting of the metal-rich, newly underplated, thin (30–40 km)hydrous juvenile crust during a tectonic transition from arc to back-arc settings.

6. Conclusions

We have established that four stages of magmatism characterizing the SCB-CR SLIP between 149–100Ma.Stage 1 consists of highly fractionated granite that emplaced at circa 149Ma, stages 2 and 3 felsic volcanicserupted at circa 128–110Ma, and stage 4 bimodal intrusive rocks emplaced at circa 100Ma. The progressivelyhigher εHf(t) and εNd(t) values from early to late stages suggest that the contribution of juvenile componentsincreased over time. The low Mg values of the Zhilingtou felsic volcanics suggest that juvenile continentalcrust was primarily involved in the generation of the parent magma. Stage 4 mafic dikes have relatively highεHf(t) and εNd(t) values and Nd, Ta, and Ti depletions, suggesting a metasomatized asthenosphericmantle source.

Figure 14. Geochemical variations versus ages of the igneous rocks in theZhilingtou deposit. (a and b) Pb contents and εHf(t) values of the Zhilingtouigneous rocks changes with the time, respectively; (b and c) distance (km)between trench and volcanic arc; (d) epithermal mineralization occurred inresponse to tectonic transition from arc to back-arc regimes.



Based on the results in this paper and previously published data, we suggest that the formation of the SCB-CRSLIP involved in three episodes of magmatism: episode 1 consists of a localized felsic arc magmatism thatoccurred along the Zhenghe-Dapu Fault in Guangdong and Fujian provinces at 170 to 140Ma, episode 2includes widespread felsic arc magmatism that developed in Zhejiang and Fujian provinces during circa140 to 110Ma, and episode 3 consists of bimodal igneous rocks that crop out mainly along the easternmostmargin of the SCB during circa 110 to 90Ma. The spatiotemporal distribution in the SCB-CR SLIP reveals thatthe initial subduction of the Izanagi plate beneath Guangdong and Fujian provinces in the SCB began duringthe Middle to Late Jurassic. Subduction then shifted northwestward beneath Zhejiang and Fujian provincesduring the Early Cretaceous and followed by an eastward subduction retreat during the late Early Cretaceousto Late Cretaceous.

Remelting of the metal-enriched juvenile lower continental crust is critical to the epithermal mineralization-related low-Mg felsic volcanics in the SCB-CR SLIP. The low LaN/YbN ratios of the felsic volcanics reflect thethin continental crust conditions, which favored the formation of the SLIP and the related large-scale epither-mal mineralization. We conclude that the change from an arc setting to a back-arc setting in the SCB-CR SLIPinduced the generation of the large-scale epithermal deposits.

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AcknowledgmentsWe sincerely thank Jie-Xiong Hua fromthe Suichang gold mine and Jia-Run Liu,Guo-Ai Xie, and Chang-Zhi Wu fromNanjing University for assistance duringfield work. We are grateful to Bing Wufor assistance with the LA-ICP-MS zirconU-Pb dating, to Wei Pu for her assistancewith the whole-rock Sr and Nd isotopemeasurements, and to Kejun Hou for hisassistance with the zircon Hf isotopemeasurements. Hu-Jun Gong fromNorthwest University is acknowledgedfor the CL imaging. We thank Kui-DongZhao, Jian-Feng Gao, and Juan Li forthoughtful discussions. We appreciateEditor Andre Revil and refereesChristophe Galerne and S. Revillon fortheir thoughtful and constructivecomments, which greatly improve themanuscript. This study was funded bythe Ministry of Science and Technologyof China (grant 2016YFC0600205),National Natural Science Foundation ofChina (grant 41402062), and theMinistry of Land and Resources of China(grant 20089935). The presented dataare available by request from thecorresponding author.

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http://dx.doi.org/10.1029/90JB02219

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