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The widespread W-(Mo)-Sn-Nb-Ta polymetallic mineralization in Southeast (SE) China is genetically associated with Mesozoic highly fractionated granitic rocks. Such rocks have enigmatic mineralogical and geochemical features, making its petrogenesis an intensely debated topic. To better understand the underlying magma evolution processes, petrography, garnet chemistry and whole-rock major and trace element data are reported for Jurassic highly fractionated granitic rocks and associated microgranite and aplitepegmatite dikes from Macao and compared with coeval similar granitic rocks from nearby areas in SE China. Despite the fact that the most evolved rocks in Macao are garnet-bearing aplite-pegmatite dikes, the existence of coeval two-mica and garnet-bearing biotite and muscovite granites displaying more evolved compositions (e.g, lower Zr/Hf ratios) indicates that the differentiation sequence reached higher degrees of fractionation at a regional scale. Although crystal fractionation played an important role, late-stage fluid/melt interactions, involving F-rich fluids, imparted specific geochemical characteristics to Macao and SE China highly fractionated granitic rocks such as the non-CHARAC (CHArge-and-RAdius-Controlled) behavior of trace elements, leading, for example, to non-chondritic Zr/Hf ratios, Rare Earth Elements (REE) tetrad effects and Nb-Ta enrichment and fractionation. Such process contributed to the late-stage crystallization of accessory phases only found in these highly evolved facies. Among the latter, two populations of garnet were identified in MGI (Macao Group I) highly fractionated granitic rocks: small grossular-poor euhedral grains and large grossular-rich skeletal garnet grains with quartz inclusions. The first group was mainly formed through precipitation from highly evolved Mn-rich slightly peraluminous melts under low-pressure and relatively low temperature (∼700 °C) conditions. Assimilation of upper crust metasedimentary materials may have contributed as a source of Mn and Al to the formation of garnet. The second group has a metasomatic origin related to the interaction of magmatic fluids with previously crystallized mineral phases and, possibly, with assimilated metasedimentary enclaves or surrounding metasedimentary strata. The highly fractionated granitic rocks in Macao represent the first stage in the development of granite-related W-(Mo)-Sn-Nb-Ta mineralization associated with coeval more evolved lithotypes in SE China.

Abstract Much controversy has occurred in the past few decades regarding the nature of the sources, the petrogenetic processes, and the tectonic regime(s) of the Jurassic magmatism within the Southeast China magmatic belt. This study aims to contribute to the discussion with mineral chemistry, and whole-rock element and Sr-Nd-Hf-Pb isotopic geochemical data from granitic rocks and microgranular mafic enclaves from Macao, where two discrete groups of I-type biotite granites have been identified (referred to as Macao Group I [MGI] and Macao Group II [MGII]). It is proposed that the granitic magmas were generated by partial melting of infracrustal medium- to high-K, basaltic Paleoproterozoic to Mesoproterozoic protoliths (Nd depleted mantle model age [TDM2] = 1.7–1.6 Ga and Hf TDM2 = 1.8–1.6 Ga), triggered by underplating of hot mantle-derived magmas in an extensional setting related to the foundering of a previously flat slab (paleo–Pacific plate) beneath the SE China continent. The main differences between the two groups of Macao granites are attributed to assimilation and fractional crystallization processes, during which upper-crustal Paleozoic metasediments were variably assimilated by MGI magmas. This is evidenced by an increase in initial 87Sr/86Sr ratios with degree of evolution, presence of metasedimentary enclaves, and high percentage of zircon xenocrysts with Paleozoic ages. In addition, other processes like late-stage fluid/melt interaction and magma mixing also left some imprints on granite compositions (rare earth element tetrad effect plus non–charge-and-radius-controlled behavior of trace elements and decoupling between different isotope systems, respectively). The distribution of isotopically distinct granites in SE China reflects the nature of the two Cathaysia crustal blocks juxtaposed along the Zhenghe-Dapu fault.

The territory of Macao is composed of several granitic intrusions belonging to one of the biggest granite provinces in the world, the Southeast China Magmatic Belt (SCMB), located in the southeast (SE) area of the Cathaysia Block. The SCMB is known by the occurrence of large volumes of Mesozoic magmatic rocks (over 90% are granitic rocks and equivalent volcanic rocks with minor basalts), occupying a total outcrop area of nearly 200.000 km2. The geology of Macao (~30 Km2) is dominated by granitic rocks displaying a wide range of textural, mineralogical and chemical features, making it an ideal region to study these rocks and the petrogenetic processes responsible for their diversity. This study employed a wide range of research methodologies, namely field studies, petrography, zircon geochronology, mineral chemistry, whole-rock elemental and isotopic geochemistry to determine the nature of the source, the petrogenetic processes and the tectonic regimes of the Mesozoic magmatism in this region. Thus, the data collected along this study aims to provide new knowledge on the tectono-magmatic evolution of Macao, in particular, and of SE China, in general. The results obtained from the high-precision U–Pb zircon geochronology, acquired through isotope dilution thermal ionization mass spectrometry (ID-TIMS) and in-situ laser ablation multi-collector inductively coupled mass spectrometry (LA-MC-ICPMS), revealed different ages for Macao granites. Despite its relatively small area, the determined ages tightly constrain the Macao granitic magmatism to two periods, ranging from 164.5 ± 0.6 to 162.9 ± 0.7 Ma (MGI – Macao Group I granites) and 156.6 ± 0.2 to 155.5 ± 0.8 Ma (MGII – Macao Group II granites). In addition, younger dacitic rocks were dated at 150.6 ± 0.6 Ma and <120 Ma. The existence of two proximal but distinct granitic pulses, spanning for a time of about 9 Ma and separated by ca. 6 Ma, in the Macao granitic suite suggests that it was incrementally assembled. This hypothesis is also extendable to the neighbouring Hong Kong region, where the magmatic activity occurred in four major pulses spanning for about 24 Ma. However, the MGII granites indicate the occurrence, on the Pearl River Delta region, of a magmatic pulse between those defined in Hong Kong at the origin of Lamma Suite (165–160 Ma) and the Kwai Chung Suite (148–146 Ma). In addition, Rare Element Earth (REE) ratios suggest that this pulse may only occur in Macao area, while MGI granites show evolving trends of REE ratios similar to those of Jurassic granites outcropping in vast areas of the Cathaysia Block (SE China). Inheritance patterns in the zircon U–Pb data indicate the presence of a population of antecrysts (165–180 Ma) crystallized from earlier magmatic pulses and a population of inherited zircons, from Precambrian to Phanerozoic sources, incorporated into the magmas during melting and/or ascent/emplacement at crustal levels. The oldest inherited ages (2.4 Ga and possibly 2.9 Ga) suggest contribution of Proterozoic and possibly of late Archaean crustal sources for the Macao magmatism. The granitic rocks of Macao are mainly high-K calc-alkaline metaluminous to weakly peraluminous I-type granites with variable degrees of fractionation. Fractional crystallization played an important role in the evolution of these granites, though the fractionation paths differ for the highly fractionated facies of both groups mainly due to distinct accessory fractionating phases. Such difference is evident by distinct REE evolution trends: while MGI magmas seem to have evolved by gradual enrichment in heavy REE relatively to light REE, originating progressively flatter REE patterns, magmas from MGII are marked by depletion of middle REE, leading to progressively concave upward REE patterns. However, while most of the geochemical variation of the MGII granites can be explained by fractional crystallization, the same is not true for MGI granites. The MGI highly fractionated granites show evidence for the REE tetrad effect and are characterized by non-CHArge-and-RAdius-Controlled (non-CHARAC) behaviour of trace elements, suggesting late-stage melt/fluid interactions involving F-rich fluids. The stage of evolution represented by the MGI highly fractionated granites corresponds to the onset of fluid/melt interaction in a highly evolved granitic system, which may have led to enhanced hydrothermal activity in more evolved stages, as those represented in neighbouring areas in SE China. Significant differences in isotopic composition were also observed, with the MGII being characterized by a much narrow range of initial 87Sr/86Sr ratios and εNd(t) and εHf(t) values than MGI. Based on these differences, the MGII granites are considered to be part of a comagmatic suite that has evolved in closed system, contrasting with what can be inferred for MGI. The increase in initial 87Sr/86Sr ratios with degree of evolution, the presence of metasedimentary enclaves and the high percentage of inherited zircon with Paleozoic ages in MGI, suggest the occurrence of an assimilation fractionation crystallization (AFC) process. The AFC processes were a major cause for the I-S transitional characteristics of the MGI highly fractionated granites and possibly of the other similar Jurassic biotite granites in SE China. The observed decoupling of Sr, Nd and Hf isotope systems might have resulted from magma mixing between the granitic and more mafic magmas, which caused the homogenization of Sr isotope ratios but not of the Nd and Hf ones. Such process is also supported by the occurrence of Microgranular Mafic Enclaves (MME) hosted by the granites. Isotope and major element compositions together with model ages strongly suggest that Macao granitic magmas were generated by partial melting of infracrustal medium-to-high K basaltic Paleo-Proterozoic to Mesoproterozoic protoliths heated by, and mixed to some degree with mantle-derived magmas. The temporal and spatial association of Macao and SE China Jurassic I-type granites with basaltic/gabbroic rocks, syenites and A-type granites, displaying typical intraplate chemical features, indicates an extensional regime rather than an active margin for the origin of these rocks. It also points to an important role of mantle-derived magmas in the production of SE China Jurassic granites. Adiabatic decompression melting of the asthenospheric mantle produced mafic magmas, which underplated at the base of the crust (Moho), subsequently triggering partial melting of the lower crust to generate the granitic magmas. The Jurassic Macao granites are interpreted as being produced in an intraplate extensional setting related to the break-off and foundering of a previously flat-slab (Paleo-Pacific plate) beneath the Eurasian plate. The boundary between east and west Cathaysia blocks is roughly along the Zhenghe-Dapu Fault (ZDF), which intersects the SE China coast near Hong Kong and is thought to have played a major role for the Mesozoic magmatic activity in this region. The stronger isotopic affinities of Macao granites with the other granitic rocks and lower crustal xenoliths from the western Cathaysia Block suggest that the ZDF is likely to pass south of Macao, a fact that has not been mentioned before. In addition to the Early Yanshanian (Jurassic) granitic magmatism in Macao, the younger ages obtained for the dacite dykes indicate that the territory was also affected, to a lesser degree, by Late Yanshanian (Cretaceous) magmatism. The transition from granitic to dacitic magmatism most likely corresponds to a change in the regional tectonic regime, which induced a significant change in the magma genesis processes. In contrast with the intraplate features of Macao and SE China Jurassic granites and coeval mafic rocks, the geochemical features of the Macao dacite dykes (e.g. high LILE/HFSE ratios and negative anomalies of Nb, Ta and Ti) are identical to those characterizing arc-like subduction-related magmas. These dacites are most likely evolved products of arc-like magmatism and may testify the reestablishment of a normal subduction system in this area of SE China.

A 1:12,000 geological map of the Macao Special Administrative Region has been produced through detailed field work supported by petrographic, mineralogical, geochronological and geochemical data obtained in previous studies. This map aims to represent a reliable tool to understand the geological evolution of the region and for management of the territory. The geology of Macao is dominated by two groups of Jurassic granitic rocks belonging to an intrusive suite located along the coast of Southeast China: Macao Group I (MGI: 164.5 ± 0.6 to 162.9 ± 0.7 Ma) and Macao Group II (MGII: 156.6 ± 0.2 to 155.5 ± 0.8 Ma), including the associated microgranite, aplite and pegmatite dikes and quartz veins. Remnants of the metasedimentary wall-rock are present as Devonian xenoliths enclosed within the granites. Younger Jurassic to Cretaceous andesite to dacite dikes (150.6 ± 0.6 to <120 Ma) intrude the granitic rocks. Additionally, Quaternary sedimentary deposits cover the older lithologies.