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Markov Chain Monte Carlo (MCMC) methods are widely used and preferred when the sampling distribution is intractable. In estimation problems with Monte Carlo samples, it is critical to quantify uncertainty of estimators on some intervals since the true function could not be obtained in most cases. Traditional pointwise confidence intervals could provide certain coverage probability in a single point but fail to provide simultaneous coverage for the whole function without a multiplicity correction. The Bonferroni method corrects for multiplicity, but these conservative intervals do not achieve the desired nominal level. This dissertation focuses on providing and quantifying the uncertainty of estimators in the form of a confidence band (CB) to increase the reliability of the resulting inferences.We begin with MCMC basics and point estimation methods. Then we provide estimators for densities and general functions separately. We discuss the covariance matrix and Central Limit Theorem as preliminary settings. Afterwards, we review pointwise and Bonferroni methods to construct CBs. We propose three methods in calculating simultaneous CBs with theories and algorithms which are followed by examples to compare the coverage probabilities and the band widths. To provide more intuitive results, we compared the bands with three simulation examples: AR(1) model, mixed normal distribution, and a general function case. Then we used four real data examples: Michigan survey example, Telescope data example, time varying model, and a Bayesian reliability model to explain our proposed simultaneous bands.

Markov Chain Monte Carlo (MCMC) methods are widely used and preferred when the sampling distribution is intractable. In estimation problems with Monte Carlo samples, it is critical to quantify uncertainty of estimators on some intervals since the true function could not be obtained in most cases. Traditional pointwise confidence intervals could provide certain coverage probability in a single point but fail to provide simultaneous coverage for the whole function without a multiplicity correction. The Bonferroni method corrects for multiplicity, but these conservative intervals do not achieve the desired nominal level. This dissertation focuses on providing and quantifying the uncertainty of estimators in the form of a confidence band (CB) to increase the reliability of the resulting inferences.We begin with MCMC basics and point estimation methods. Then we provide estimators for densities and general functions separately. We discuss the covariance matrix and Central Limit Theorem as preliminary settings. Afterwards, we review pointwise and Bonferroni methods to construct CBs. We propose three methods in calculating simultaneous CBs with theories and algorithms which are followed by examples to compare the coverage probabilities and the band widths. To provide more intuitive results, we compared the bands with three simulation examples: AR(1) model, mixed normal distribution, and a general function case. Then we used four real data examples: Michigan survey example, Telescope data example, time varying model, and a Bayesian reliability model to explain our proposed simultaneous bands.

U−Pb geochronology of calcite using laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) is an emerging method, with potential applications to a vast array of geological problems. Due to the low levels of U and Pb in calcite, measurement using higher-sensitivity instruments, such as sector field (SF) ICP-MS, have advantages over more commonly used quadrupole (Q) ICP-MS instruments. Using a Thermo Element XR ICP-MS, we demonstrate that the Jet+X cone combination with the N2 enhancement technique provides the best sensitivity for measuring U and Pb isotopes. This higher sensitivity improves the precision of calcite U−Pb isotope measurements, and permits dating at high spatial resolutions (<110 µm) and for samples containing low contents of 238U (<1 µg g−1) and/or 207Pb (i.e., young samples <10 Ma). Using a spot size of 85 µm with a low fluence (∼2.0 J cm−2), the laser-induced elemental fractionation of 206Pb/238U in the NIST SRM 614, ARM-3 and WC-1 reference materials are insignificant (<2.2%). Adopting the optimized instrument parameters, we analysed four commonly-used calcite U−Pb reference materials (WC-1, Duff Brown Tank, JT, and ASH-15). The results match well with published isotope dilution data, demonstrating the reliability of our technique. ARM-3, an andesitic glass, is shown to be an appropriate reference material for both 207Pb/206Pb calibration and instrument optimization because of its moderate contents of U (∼3.75 µg g−1) and Pb (∼12.7 µg g−1). We further demonstrate that the image-guided approach using LA-ICP-MS elemental mapping is an efficient tool in obtaining robust ages.

While attention has been an increasingly popular component in deep neural networks to both interpret and boost the performance of models, little work has examined how attention progresses to accomplish a task and whether it is reasonable. In this work, we propose an Attention with Reasoning capability (AiR) framework that uses attention to understand and improve the process leading to task outcomes. We first define an evaluation metric based on a sequence of atomic reasoning operations, enabling a quantitative measurement of attention that considers the reasoning process. We then collect human eye-tracking and answer correctness data, and analyze various machine and human attention mechanisms on their reasoning capability and how they impact task performance. To improve the attention and reasoning ability of visual question answering models, we propose to supervise the learning of attention progressively along the reasoning process and to differentiate the correct and incorrect attention patterns. We demonstrate the effectiveness of the proposed framework in analyzing and modeling attention with better reasoning capability and task performance. The code and data are available at https://github.com/szzexpoi/AiR, Comment: To be published in TPAMI. arXiv admin note: substantial text overlap with arXiv:2007.14419

U−Pb geochronology of calcite using laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) is an emerging method, with potential applications to a vast array of geological problems. Due to the low levels of U and Pb in calcite, measurement using higher-sensitivity instruments, such as sector field (SF) ICP-MS, have advantages over more commonly used quadrupole (Q) ICP-MS instruments. Using a Thermo Element XR ICP-MS, we demonstrate that the Jet+X cone combination with the N2 enhancement technique provides the best sensitivity for measuring U and Pb isotopes. This higher sensitivity improves the precision of calcite U−Pb isotope measurements, and permits dating at high spatial resolutions (<110 µm) and for samples containing low contents of 238U (<1 µg g−1) and/or 207Pb (i.e., young samples <10 Ma). Using a spot size of 85 µm with a low fluence (∼2.0 J cm−2), the laser-induced elemental fractionation of 206Pb/238U in the NIST SRM 614, ARM-3 and WC-1 reference materials are insignificant (<2.2%). Adopting the optimized instrument parameters, we analysed four commonly-used calcite U−Pb reference materials (WC-1, Duff Brown Tank, JT, and ASH-15). The results match well with published isotope dilution data, demonstrating the reliability of our technique. ARM-3, an andesitic glass, is shown to be an appropriate reference material for both 207Pb/206Pb calibration and instrument optimization because of its moderate contents of U (∼3.75 µg g−1) and Pb (∼12.7 µg g−1). We further demonstrate that the image-guided approach using LA-ICP-MS elemental mapping is an efficient tool in obtaining robust ages.

In the present work, a natural zircon megacryst SA02 (the exact provenance unknown) is investigated as a new potential reference material for U–Pb geochronology and Hf–O isotopic composition analysis via micro-beam methods. The precise and accurate U–Pb age is determined by the chemical abrasion isotope dilution thermal ionization mass-spectrometry (CA-ID-TIMS) method. The resultant mean 206Pb/238U date is 535.10 ± 0.24 Ma (2s, n = 2), interpreted as the crystallization age of the zircon megacryst. The mean ID-TIMS 206Pb/238U date of 533.7 ± 3.7 Ma (2s, n = 8) is recommended as the working value for micro-beam analyses when using untreated SA02 zircon grains as the primary reference material. 206Pb/238U dates of 533.0 ± 6.2 Ma (2s, n = 57) and 534 ± 8 Ma (2s, n = 101) obtained by secondary ion mass spectrometry (SIMS) and laser ablation-inductively coupled plasma mass spectrometry (LA-ICP-MS) respectively are reproducible and in agreement with the results of ID-TIMS within < 0.3% relative analytical errors. Solution data of Hf isotope compositions measured by multi-collector ICP-MS (MC-ICP-MS) from SA02 zircon yield a mean 176Hf/177Hf of 0.282287 ± 0.000016 (2s, n = 31), which is recommended as a reference value for microbeam analysis. Hf isotope analyses by LA-MC-ICP-MS yield homogeneous Hf isotopic compositions with a mean 176Hf/177Hf of 0.282289 ± 0.000033 (2s, n = 142) identical to the solution value. The mean δ18O value measured by laser fluorination is 6.03 ± 0.28‰ (2s, n = 13), which is consistent with the result of SIMS analysis.

While attention has been an increasingly popular component in deep neural networks to both interpret and boost performance of models, little work has examined how attention progresses to accomplish a task and whether it is reasonable. In this work, we propose an Attention with Reasoning capability (AiR) framework that uses attention to understand and improve the process leading to task outcomes. We first define an evaluation metric based on a sequence of atomic reasoning operations, enabling quantitative measurement of attention that considers the reasoning process. We then collect human eye-tracking and answer correctness data, and analyze various machine and human attentions on their reasoning capability and how they impact task performance. Furthermore, we propose a supervision method to jointly and progressively optimize attention, reasoning, and task performance so that models learn to look at regions of interests by following a reasoning process. We demonstrate the effectiveness of the proposed framework in analyzing and modeling attention with better reasoning capability and task performance. The code and data are available at https://github.com/szzexpoi/AiR, Comment: ECCV2020 (Oral), supplementary materials included

Artificial photosystems are advanced by the development of conformal catalytic materials that promote desired chemical transformations, while also maintaining stability and minimizing parasitic light absorption for integration on surfaces of semiconductor light absorbers. Here, we demonstrate that multifunctional, nanoscale catalysts that enable high-performance photoelectrochemical energy conversion can be engineered by plasma-enhanced atomic layer deposition. The collective properties of tailored Co3O4/Co(OH)2 thin films simultaneously provide high activity for water splitting, permit efficient interfacial charge transport from semiconductor substrates, and enhance durability of chemically sensitive interfaces. These films comprise compact and continuous nanocrystalline Co3O4 spinel that is impervious to phase transformation and impermeable to ions, thereby providing effective protection of the underlying substrate. Moreover, a secondary phase of structurally disordered and chemically labile Co(OH)2 is introduced to ensure a high concentration of catalytically active sites. Application of this coating to photovoltaic p+n-Si junctions yields best reported performance characteristics for crystalline Si photoanodes.

Artificial photosystems are advanced by the development of conformal catalytic materials that promote desired chemical transformations, while also maintaining stability and minimizing parasitic light absorption for integration on surfaces of semiconductor light absorbers. Here, we demonstrate that multifunctional, nanoscale catalysts that enable high-performance photoelectrochemical energy conversion can be engineered by plasma-enhanced atomic layer deposition. The collective properties of tailored Co3O4/Co(OH)2 thin films simultaneously provide high activity for water splitting, permit efficient interfacial charge transport from semiconductor substrates, and enhance durability of chemically sensitive interfaces. These films comprise compact and continuous nanocrystalline Co3O4 spinel that is impervious to phase transformation and impermeable to ions, thereby providing effective protection of the underlying substrate. Moreover, a secondary phase of structurally disordered and chemically labile Co(OH)2 is introduced to ensure a high concentration of catalytically active sites. Application of this coating to photovoltaic p+n-Si junctions yields best reported performance characteristics for crystalline Si photoanodes.

Iridium oxide is one of the few catalysts capable of catalyzing the oxygen evolution reaction (OER) in both acidic and basic conditions. Understanding the mechanism of IrOx under realistic photoelectrochemical conditions is important for the development of integrated water-splitting systems. Herein, we have developed a highly efficient OER photoanode in pH 1 aqueous solutions based on a sputtered IrOx film and a p(+)n-Si light absorber, interfaced with a sputtered Au layer. Operando high-energy-resolution fluorescence detection X-ray absorption spectroscopy (HERFD XAS) was employed to monitor the oxidation state changes of IrOx during both electrochemical and photoelectrochemical (PEC) water oxidation reactions in pH 1 aqueous solutions. We observed a gradual increase of the average oxidation state of Ir with increasing anodic potential in the precatalytic region, followed by a reduction of Ir under O-2 evolution conditions. Consistent results were obtained on dark anodes and illuminated photoanodes. However, when the thickness of IrO2 was increased to 2 and 3 nm, the spectral changes became much less pronounced, and the reduction of Ir oxidation state after the OER onset was not observed. This is due to the lower surface-to-bulk ratio, where lattice oxygen sites in the bulk are not accessible for the formation of hydroxide. More generally, the operando method developed here can be extended to other materials, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.

Photoelectrochemical water splitting is a promising approach for renewable production of hydrogen from solar energy and requires interfacing advanced water-splitting catalysts with semiconductors. Understanding the mechanism of function of such electrocatalysts at the atomic scale and under realistic working conditions is a challenging, yet important, task for advancing efficient and stable function. This is particularly true for the case of oxygen evolution catalysts and, here, we study a highly active Co3O4/Co(OH)2 biphasic electrocatalyst on Si by means of operando ambient-pressure X-ray photoelectron spectroscopy performed at the solid/liquid electrified interface. Spectral simulation and multiplet fitting reveal that the catalyst undergoes chemical-structural transformations as a function of the applied anodic potential, with complete conversion of the Co(OH)2 and partial conversion of the spinel Co3O4 phases to CoO(OH) under precatalytic electrochemical conditions. Furthermore, we observe new spectral features in both Co 2p and O 1s core-level regions to emerge under oxygen evolution reaction conditions on CoO(OH). The operando photoelectron spectra support assignment of these newly observed features to highly active Co4+ centers under catalytic conditions. Comparison of these results to those from a pure phase spinel Co3O4 catalyst supports this interpretation and reveals that the presence of Co(OH)2 enhances catalytic activity by promoting transformations to CoO(OH). The direct investigation of electrified interfaces presented in this work can be extended to different materials under realistic catalytic conditions, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.

Photoelectrochemical water splitting is a promising approach for renewable production of hydrogen from solar energy and requires interfacing advanced water-splitting catalysts with semiconductors. Understanding the mechanism of function of such electrocatalysts at the atomic scale and under realistic working conditions is a challenging, yet important, task for advancing efficient and stable function. This is particularly true for the case of oxygen evolution catalysts and, here, we study a highly active Co3O4/Co(OH)2 biphasic electrocatalyst on Si by means of operando ambient-pressure X-ray photoelectron spectroscopy performed at the solid/liquid electrified interface. Spectral simulation and multiplet fitting reveal that the catalyst undergoes chemical-structural transformations as a function of the applied anodic potential, with complete conversion of the Co(OH)2 and partial conversion of the spinel Co3O4 phases to CoO(OH) under precatalytic electrochemical conditions. Furthermore, we observe new spectral features in both Co 2p and O 1s core-level regions to emerge under oxygen evolution reaction conditions on CoO(OH). The operando photoelectron spectra support assignment of these newly observed features to highly active Co4+ centers under catalytic conditions. Comparison of these results to those from a pure phase spinel Co3O4 catalyst supports this interpretation and reveals that the presence of Co(OH)2 enhances catalytic activity by promoting transformations to CoO(OH). The direct investigation of electrified interfaces presented in this work can be extended to different materials under realistic catalytic conditions, thereby providing a powerful tool for mechanism discovery and an enabling capability for catalyst design.

Artificial photosynthesis relies on the availability of semiconductors that are chemically stable and can efficiently capture solar energy. Although metal oxide semiconductors have been investigated for their promise to resist oxidative attack, materials in this class can suffer from chemical and photochemical instability. Here we present a methodology for evaluating corrosion mechanisms and apply it to bismuth vanadate, a state-of-the-art photoanode. Analysis of changing morphology and composition under solar water splitting conditions reveals chemical instabilities that are not predicted from thermodynamic considerations of stable solid oxide phases, as represented by the Pourbaix diagram for the system. Computational modelling indicates that photoexcited charge carriers accumulated at the surface destabilize the lattice, and that self-passivation by formation of a chemically stable surface phase is kinetically hindered. Although chemical stability of metal oxides cannot be assumed, insight into corrosion mechanisms aids development of protection strategies and discovery of semiconductors with improved stability.

The ca. 3480-3430 Ma Tsawela Gneiss (TG) is a well-preserved coarse-grained diorite to tonalite suite within the Ancient Gneiss Complex of Swaziland, eastern Kaapvaal craton. These gneisses are texturally and compositionally distinct from the hosting oldest components of the ca. 3200-3660 Ma TTG-type Ngwane Gneisses (NG). Major and trace elements, in combination with whole-rock hafnium-neodymium isotopic data, were analyzed in the TG and in three samples of ca. 3450 Ma grey NG to constrain sources and magmatic processes. High-field-strength element data (HFSE) were combined with U-Pb SHRIMP II ages and Hf-in-zircon data for key samples to constrain their ages and petrogenesis. In contrast to the widespread view that Archaean crust is mainly composed of TTG igneous suites that formed from juvenile sources, the geochemical and isotopic compositions of the TG indicate that these rocks represent a calc-alkaline plutonic suite which possibly formed by magma mixing processes involving juvenile, mantle-derived tholeiitic melts as well as partial melts of the older Ngwane gneiss. Alternatively, the TG may represent a magmatic suite that formed by fractional crystallization of a hydrous intermediate magma. These results contrast with field evidence of a relatively uniform and homogeneous composition. Our geochronological and isotopic data show that the TG intruded the NG during a time span of at least 50 Ma without any significant compositional change of the source. The predominant influence of fractional crystallization of a tholeiitic mafic magma, as well as assimilation-fractional-crystallization processes (AFC) can be excluded for the TG from major and trace element modelling. The magma processes proposed here suggest efficient mixing of approximately equal amounts of TG magmas with those derived from the NG basement and is supported by the largely homogeneous Hf-Nd isotopic compositions of the whole-rock samples. We propose that melting and mixing occurred in the lower

Artificial photosynthesis relies on the availability of semiconductors that are chemically stable and can efficiently capture solar energy. Although metal oxide semiconductors have been investigated for their promise to resist oxidative attack, materials in this class can suffer from chemical and photochemical instability. Here we present a methodology for evaluating corrosion mechanisms and apply it to bismuth vanadate, a state-of-the-art photoanode. Analysis of changing morphology and composition under solar water splitting conditions reveals chemical instabilities that are not predicted from thermodynamic considerations of stable solid oxide phases, as represented by the Pourbaix diagram for the system. Computational modelling indicates that photoexcited charge carriers accumulated at the surface destabilize the lattice, and that self-passivation by formation of a chemically stable surface phase is kinetically hindered. Although chemical stability of metal oxides cannot be assumed, insight into corrosion mechanisms aids development of protection strategies and discovery of semiconductors with improved stability.

The ca. 3480-3430 Ma Tsawela Gneiss (TG) is a well-preserved coarse-grained diorite to tonalite suite within the Ancient Gneiss Complex of Swaziland, eastern Kaapvaal craton. These gneisses are texturally and compositionally distinct from the hosting oldest components of the ca. 3200-3660 Ma TTG-type Ngwane Gneisses (NG). Major and trace elements, in combination with whole-rock hafnium-neodymium isotopic data, were analyzed in the TG and in three samples of ca. 3450 Ma grey NG to constrain sources and magmatic processes. High-field-strength element data (HFSE) were combined with U-Pb SHRIMP II ages and Hf-in-zircon data for key samples to constrain their ages and petrogenesis. In contrast to the widespread view that Archaean crust is mainly composed of TTG igneous suites that formed from juvenile sources, the geochemical and isotopic compositions of the TG indicate that these rocks represent a calc-alkaline plutonic suite which possibly formed by magma mixing processes involving juvenile, mantle-derived tholeiitic melts as well as partial melts of the older Ngwane gneiss. Alternatively, the TG may represent a magmatic suite that formed by fractional crystallization of a hydrous intermediate magma. These results contrast with field evidence of a relatively uniform and homogeneous composition. Our geochronological and isotopic data show that the TG intruded the NG during a time span of at least 50 Ma without any significant compositional change of the source. The predominant influence of fractional crystallization of a tholeiitic mafic magma, as well as assimilation-fractional-crystallization processes (AFC) can be excluded for the TG from major and trace element modelling. The magma processes proposed here suggest efficient mixing of approximately equal amounts of TG magmas with those derived from the NG basement and is supported by the largely homogeneous Hf-Nd isotopic compositions of the whole-rock samples. We propose that melting and mixing occurred in the lower

Achieving stable operation of photoanodes used as components of solar water splitting devices is critical to realizing the promise of this renewable energy technology. It is shown that p-type transparent conducting oxides (p-TCOs) can function both as a selective hole contact and corrosion protection layer for photoanodes used in light-driven water oxidation. Using NiCo2O4 as the p-TCO and n-type Si as a prototypical light absorber, a rectifying heterojunction capable of light driven water oxidation was created. By placing the charge separating junction in the Si using a np(+) structure and by incorporating a highly active heterogeneous Ni-Fe oxygen evolution catalyst, efficient light-driven water oxidation can be achieved. In this structure, oxygen evolution under AM1.5G illumination occurs at 0.95 V vs RHE, and the current density at the reversible potential for water oxidation (1.23 V vs RHE) is >25 mA cm(-2). Stable operation was confirmed by observing a constant current density over 72 h and by sensitive measurements of corrosion products in the electrolyte. In situ Raman spectroscopy was employed to investigate structural transformation of NiCo2O4 during electrochemical oxidation. The interface between the light absorber and p-TCO is crucial to produce selective hole conduction to the surface under illumination. For example, annealing to produce more crystalline NiCo2O4 produces only small changes in its hole conductivity, while a thicker SiOx layer is formed at the n-Si/p-NiCo2O4 interface, greatly reducing the PEC performance. The generality of the p-TCO protection approach is demonstrated by multihour, stable, water oxidation with n-InP/p-NiCo2O4 heterojunction photoanodes.

Achieving stable operation of photoanodes used as components of solar water splitting devices is critical to realizing the promise of this renewable energy technology. It is shown that p-type transparent conducting oxides (p-TCOs) can function both as a selective hole contact and corrosion protection layer for photoanodes used in light-driven water oxidation. Using NiCo2O4 as the p-TCO and n-type Si as a prototypical light absorber, a rectifying heterojunction capable of light driven water oxidation was created. By placing the charge separating junction in the Si using a np(+) structure and by incorporating a highly active heterogeneous Ni-Fe oxygen evolution catalyst, efficient light-driven water oxidation can be achieved. In this structure, oxygen evolution under AM1.5G illumination occurs at 0.95 V vs RHE, and the current density at the reversible potential for water oxidation (1.23 V vs RHE) is >25 mA cm(-2). Stable operation was confirmed by observing a constant current density over 72 h and by sensitive measurements of corrosion products in the electrolyte. In situ Raman spectroscopy was employed to investigate structural transformation of NiCo2O4 during electrochemical oxidation. The interface between the light absorber and p-TCO is crucial to produce selective hole conduction to the surface under illumination. For example, annealing to produce more crystalline NiCo2O4 produces only small changes in its hole conductivity, while a thicker SiOx layer is formed at the n-Si/p-NiCo2O4 interface, greatly reducing the PEC performance. The generality of the p-TCO protection approach is demonstrated by multihour, stable, water oxidation with n-InP/p-NiCo2O4 heterojunction photoanodes.

We report zircon ages, Hf-in-zircon isotopes as well as whole-rock geochemistry and Hf-Nd isotopic systematics for Palaeoarchaean grey gneisses of the Ancient Gneiss Complex of Swaziland, the oldest components of the Kaapvaal craton, southern Africa. The Hf-in-zircon isotopic compositions in these compositionally heterogeneous, multicomponent, migmatitic gneisses are highly variable, even in the oldest zircons dating back to 3.66 Ga, suggesting growth of zircon from melts representing a mix of juvenile and anatectic material derived from differentiated continental crust of Eoarchean to late Hadean age. In contrast, the initial Nd and Hf whole-rock isotopic compositions are frequently not in agreement with the Hf-in-zircon data that mostly show approximately chondritic initial values for Nd and strongly radiogenic initial values for Hf. We consider it likely that both the Lu-Hf and Sm-Nd whole-rock isotopic systems were disturbed and partly reset during later episodes of partial melting and crustal reworking, most likely during a pervasive 3.2 Ga tectono-metamorphic event. Primitive mantle-normalized trace element patterns show the variable influence of residual plagioclase and garnet in the sources as well as high contents of strongly incompatible elements. In conjunction with the Hf-in-zircon isotopic data the trace element contents are best explained by the incorporation of older continental crustal material into the sources of the grey gneisses. Our data support evidence from other Palaeoarchean terranes that crustal recycling, as seen in even the oldest crustal components, played an important role in early continental evolution. Rocks previously classified as a subduction-related tonalite-trondhjemite-granodiorite suite are complex, and their chemistry alone cannot be used to reconstruct tectonic settings. (C) 2014 Elsevier B.V. All rights reserved.

We report zircon ages, Hf-in-zircon isotopes as well as whole-rock geochemistry and Hf-Nd isotopic systematics for Palaeoarchaean grey gneisses of the Ancient Gneiss Complex of Swaziland, the oldest components of the Kaapvaal craton, southern Africa. The Hf-in-zircon isotopic compositions in these compositionally heterogeneous, multicomponent, migmatitic gneisses are highly variable, even in the oldest zircons dating back to 3.66 Ga, suggesting growth of zircon from melts representing a mix of juvenile and anatectic material derived from differentiated continental crust of Eoarchean to late Hadean age. In contrast, the initial Nd and Hf whole-rock isotopic compositions are frequently not in agreement with the Hf-in-zircon data that mostly show approximately chondritic initial values for Nd and strongly radiogenic initial values for Hf. We consider it likely that both the Lu-Hf and Sm-Nd whole-rock isotopic systems were disturbed and partly reset during later episodes of partial melting and crustal reworking, most likely during a pervasive 3.2 Ga tectono-metamorphic event. Primitive mantle-normalized trace element patterns show the variable influence of residual plagioclase and garnet in the sources as well as high contents of strongly incompatible elements. In conjunction with the Hf-in-zircon isotopic data the trace element contents are best explained by the incorporation of older continental crustal material into the sources of the grey gneisses. Our data support evidence from other Palaeoarchean terranes that crustal recycling, as seen in even the oldest crustal components, played an important role in early continental evolution. Rocks previously classified as a subduction-related tonalite-trondhjemite-granodiorite suite are complex, and their chemistry alone cannot be used to reconstruct tectonic settings. (C) 2014 Elsevier B.V. All rights reserved.

Colloidal MoS2 nanoparticles with diameters of less than 10 nm were prepared with a simple solvothermal method and demonstrated high efficiency in catalyzing H-2 evolution in Ru(bpy)(3)(2+)-based molecular systems under visible light., QC 20100525

Sm-Nd isotope data indicate that mineralising materials for the large vein deposit, in Shandong, were derived from the host Mesozoic granitoids and from porphyry mafic dykes that intrude the granitoids. The gold mineralisation is more than 10 m.y. younger than the granitoids, suggesting that the mineralising fluids were meteoric rather than magmatic., Sm-Nd isotope data indicate that mineralising materials for the large vein deposit, in Shandong, were derived from the host Mesozoic granitoids and from porphyry mafic dykes that intrude the granitoids. The gold mineralisation is more than 10 m.y. younger than the granitoids, suggesting that the mineralising fluids were meteoric rather than magmatic.

The hydrothermal lode deposit is located along the outside contact of the Guojialing granodiorite. The veins contain pyrite, quartz, chalcopyrite, galena, pyrrhotite and sphalerite, of which pyrite and quartz are the main Au-bearing minerals. The micro-components of pyrite at the stages before and during gold mineralisation were investigated by scanning electron microscopy with EDS and the zoning and distribution of Au and Ag were used to consider the genesis of the Au-bearing pyrite., The hydrothermal lode deposit is located along the outside contact of the Guojialing granodiorite. The veins contain pyrite, quartz, chalcopyrite, galena, pyrrhotite and sphalerite, of which pyrite and quartz are the main Au-bearing minerals. The micro-components of pyrite at the stages before and during gold mineralisation were investigated by scanning electron microscopy with EDS and the zoning and distribution of Au and Ag were used to consider the genesis of the Au-bearing pyrite.