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Funding Information: This project was primarily supported by the National Key R&D Program of China (Grant 2018YFA0307200), the National Natural Science Foundation of China (Grants 91950119, 61905196, and 62090033), Key Research and Development Program in Shaanxi Province of China (Grant 2020JZ-10), and the Fundamental Research Funds for the Central Universities (Grants 310201911cx032, 3102019JC008, and D5000210905). The authors also thank the Analytical & Testing Center of NPU for their assistance in device fabrication and characterizations. Publisher Copyright: © 2022 American Chemical Society. Two-dimensional (2D) materials, featuring distinctive electronic and optical properties and dangling-bond-free surfaces, are promising for developing high-performance on-chip photodetectors in photonic integrated circuits. However, most of the previously reported devices operating in the photoconductive mode suffer from a high dark current or a low responsivity. Here, we demonstrate a MoTe2p-i-n homojunction fabricated directly on a silicon photonic crystal (PC) waveguide, which enables on-chip photodetection with ultralow dark current, high responsivity, and fast response speed. The adopted silicon PC waveguide is electrically split into two individual back gates to selectively dope the top regions of the MoTe2 channel in p- or n-types. High-quality reconfigurable MoTe2 (p-i-n, n-i-p, n-i-n, p-i-p) homojunctions are realized successfully, presenting rectification behaviors with ideality factors approaching 1.0 and ultralow dark currents less than 90 pA. Waveguide-assisted MoTe2 absorption promises a sensitive photodetection in the telecommunication O-band from 1260 to 1340 nm, though it is close to MoTe2's absorption band-edge. A competitive photoresponsivity of 0.4 A/W is realized with a light on/off current ratio exceeding 104 and a record-high normalized photocurrent-to-dark-current ratio of 106 mW-1. The ultrasmall capacitance of p-i-n homojunction and high carrier mobility of MoTe2 promise a high dynamic response bandwidth close to 34.0 GHz. The proposed device geometry has the advantages of employing a silicon PC waveguide as the back gates to build a 2D material p-i-n homojunction directly and simultaneously to enhance light-2D material interaction. It provides a potential pathway to develop 2D material-based photodetectors, laser diodes, and electro-optic modulators on silicon photonic chips.

Building a reliable relationship between the electronic structure of alloyed metallic catalysts and catalytic performance is important but remains challenging due to the interference from many entangled factors. Herein, a PdBi surface alloy structural model, by tuning the deposition rate of Bi atoms relative to the atomic interdiffusion rate at the interface, realizes a continuous modulation of the electronic structure of Pd. Using advanced X-ray characterization techniques, we provide a precise depiction of the electronic structure of the PdBi surface alloy. As a result, the PdBi catalysts show enhanced propene selectivity compared with the pure Pd catalyst in the selective hydrogenation of propyne. The prevented formation of saturated β-hydrides in the subsurface layers and weakened propene adsorption on the surface contribute to the high selectivity. Our work provides in-depth understanding of the electronic properties of surface alloy structure and underlies the study of the electronic structure-performance relationship in bimetallic catalysts.

The instability of perovskite nanocrystals (NCs) to moisture, heat, and blue light severely hinders their commercial applications in quantum dot displays. Here, organic semiconducting molecules are introduced onto CsPbBr

Two-dimensional (2D) materials, featuring distinctive electronic and optical properties and dangling-bond-free surfaces, are promising for developing high-performance on-chip photodetectors in photonic integrated circuits. However, most of the previously reported devices operating in the photoconductive mode suffer from a high dark current or a low responsivity. Here, we demonstrate a MoTe

Lead halide perovskite nanocrystals (CsPbX3 NCs) have been regarded as promising materials in photocatalysis. Combining metal single atoms with CsPbX3 NCs may be a practical way in exploring perovskite-based catalysts. However, such hybrids have not been achieved experimentally yet, mainly due to the weak interaction between the metal atom and the CsPbX3 surface. Here, we demonstrate that Pt single atoms can be deposited on CsPbBr3 NCs through a photoassisted approach, in which the surface was partially oxidized first, followed by the anchoring of Pt single atoms through the formation of Pt-O and Pt-Br bonds. The deposition of Pt single atoms can significantly change the photophysical properties of CsPbBr3 NCs by inducing the generation of deep trap states in the band gap. The as-prepared Pt-SA/CsPbBr3 can be used as efficient and durable catalysts for photocatalytic semi-hydrogenation of propyne. A CsPbBr3 nanocrystal might be a suitable substrate for anchoring other metal single atoms, such as Cu, Au, Ag, Pd, and so on.

A facile strategy for the preparation of a nanoconfined Ti3C2/Ru cocatalyst by direct reduction of Ru3+ ions without an additional reductant was developed. The in situ formation of TiO2 nanosheets on the Ti3C2/Ru surface ensures the separation of the semiconductor and cocatalyst (TiO2-Ti3C2/Ru), resulting in charge segregation and migration more effective than those achieved by traditionally prepared Ru-TiO2-Ti3C2. Owing to its low Fermi level, the self-assembled Ti3C2/Ru cocatalyst accepted the photogenerated electrons and promoted H2 evolution without an induction period, while exhibiting high surface structure stability. The changes in the work function and surface terminations of Ti3C2 during the photocatalysis were revealed by DFT calculations and in situ diffuse reflectance infrared Fourier transform spectroscopy. The efficient electron transfer enabled by the structurally separated Ti3C2/Ru-based photocatalyst significantly reduced the electron-hole recombination, increasing the photocatalytic H2 evolution activity. This work provides a guiding design approach for future solar energy conversion with the semiconductor-cocatalyst system.

Plasmonic nanomaterials with strong absorption at near-infrared frequencies are promising photothermal therapy agents (PTAs). The pursuit of high photothermal conversion efficiency has been the central focus of this research field. Here, we report the development of plasmonic nanoparticle clusters (PNCs) as highly efficient PTAs and provide a semiquantitative approach for calculating their resonant frequency and absorption efficiency by combining the effective medium approximation (EMA) theory and full-wave electrodynamic simulations. Guided by the theoretical prediction, we further develop a universal strategy of space-confined seeded growth to prepare various PNCs. Under optimized growth conditions, we achieve a record photothermal conversion efficiency of up to ∼84% for gold-based PNCs, which is attributed to the collective plasmon-coupling-induced near-unity absorption efficiency. We further demonstrate the extraordinary photothermal therapy performance of the optimized PNCs iniin vivo/iapplication. Our work demonstrates the high feasibility and efficacy of PNCs as nanoscale PTAs.

Fabricating CsPbX3-based heterostructures has proven to be a feasible way to tune their photophysical properties. Here, we report the successful fabrication of Janus CsPbX3/ZrO2 heterostructure nanocrystals (NCs), in which each CsPbX3 NC is partially covered by ZrO2. According to the band alignment, CsPbBr3/ZrO2 and CsPbI3/ZrO2 can be indexed as type I and type II composites, respectively. The type I composites display great enhancement in photoluminescence quantum yield (from 63 to 90%) and photoluminescence lifetime (from 12.9 to 66.1 ns) because of the charge carrier confinement and passivation effect provided by ZrO2. In contrast, the type II composites can be used in photocatalytic reduction of CO2 because electrons and holes are effectively separated and accumulated in ZrO2 and CsPbI3, respectively, under irradiation. Janus CsPbBr3/ZrO2 NCs showed a stability much higher than that of pristine CsPbBr3 against polar solvent treatment. A stable and highly efficient light-emitting device with luminous e...

The recent advancements in interfacial evaporation of salty water using renewable solar energy provide one of the promising pathways to solve worldwide water scarcity. Pursuing a stable evaporation rate of water has been the central focus of this field, as it is directly related to the throughput, while salt deposition on the evaporator becomes a critical issue. Although Janus-structured evaporators with an upper hydrophobic layer and a bottom hydrophilic layer have been demonstrated as an effective way to suppress the salt precipitation, the hydrophobic upper layer, achieved usually by some special organic groups, suffers from a photochemical oxidation when exposed to oxidative chemicals in water and high-energy light, resulting in a deteriorated surface hydrophobicity. Here, we report our design of an efficient salt-rejecting Janus evaporator by taking advantage of the self-recovering surface hydrophobicity of poly(dimethylsiloxane) (PDMS) against photochemical damages, which ensures a long-term surface hydrophobicity. With its upper layer partially covered with PDMS, the Janus evaporator demonstrates an excellent salt rejection capability and exhibits a stable evaporation rate of 1.38 kg·m-2·h-1 under 1 sun illumination for 400 min of continuous operation, or 90 d of intermittent work. By combining the advantages of high structural integration, long-term salt-rejection, and efficient evaporation, our Janus evaporator holds great promise for the stable production of clean water from seawater.

A facile strategy for the preparation of a nanoconfined Ti

The practical applications of CsPbX3 nanocrystals (NCs) have been limited by their poor stability. Although much effort has been devoted to making core–shell nanostructures to enhance the stability of CsPbX3 NCs, it is still very difficult to coat CsPbX3 NCs with another material on a single-particle level. In this work, we report a facile one-pot approach to synthesize CsPbBr3@SiO2 core–shell nanoparticles (NPs), in which each core–shell NP has only one CsPbBr3 NC. The formation process has been carefully monitored. It has been found that the formation rates, determined by reaction temperature, precursor species, pH value, etc., of both CsPbBr3 and SiO2 are critical for the successful preparation of core–shell NPs. Thanks to the protection of SiO2 shell, the product shows much higher long-term stability in humid air and enhanced stability against ultrasonication treatment in water than that of naked CsPbBr3 NCs. This work not only provides a robust method for the preparation of core–shell nanostructures ...

Fabricating CsPbX

Reversible self-assembly of nanoparticles into ordered structures is essential for both fundamental study and practical applications. Although extensive work has been conducted, the demand for simple, cheap, reversible, and versatile ordering methods is still a central issue in current nanoscience and nanotechnology. Here we report a reversible and precise self-assembly of nanoparticles through a linker-free and fast approach by manipulating the interparticle forces, e.g., van der Waals (VDW) force and electrostatic force. Because VDW force is nondirectional, an oriented interaction is achieved to induce the directional binding of nanoparticles utilizing the Janus nanostructure. An effective sol-gel approach has been developed to synthesize metal-organosilica Janus nanoparticles. Dimers and trimers can be obtained by tuning the steric hindrance. After assembly, "hot-spots" can be generated between adjacent nanoparticles, and dramatic enhancement has been observed in surface-enhanced Raman scattering. The present strategy overcomes several limitations of existing approaches and allows the controlled assembly of small particles into various structures.

The practical applications of CsPbX

The well-known photochemical and thermal methods for silver nanoplate synthesis have been generally regarded as two parallel processes without strong connections. Here we report a surprising finding that both visible light and ambient O2, which are critically important in the photochemical process, also play determining roles in the thermal synthesis. By designing a series of control experiments, we reveal that the typical thermal synthesis is essentially a modified photochemical synthesis coupled with the unique redox properties of H2O2. Light irradiation and dissolved O2 are found to be essential for initiating the formation of nanoplates, but the continued growth of nanoplates is supported by the oxidative etching and subsequent reduction of Ag due to H2O2. O2 resulting from the catalytic decomposition of H2O2 etches small nanoparticles to produce Ag(+) ions, which are then reduced back to Ag(0) by anions of H2O2 to support the growth of nanoplate seeds. The involvement of H2O2 in the reaction significantly speeds up the nanoplate formation process. These findings not only greatly improve our understanding of the unique functions of H2O2 in the thermal synthesis, but also bridge the two well established synthesis processes with a unified mechanism, and significantly enhance the reproducibility of the thermal synthesis of Ag nanoplates by identifying the critical importance of ambient light and O2.

Selective growth/etching of hybrid materials is very important for the rational synthesis of hierarchical structures and precise modulation of their physical properties. Here, the lateral etching of the core-shell Au@Ag nanorods is achieved by FeCl(3) at room temperature, producing a number of dumbbell-like Ag-tipped Au nanorods. This selective etching at the side of the core-shell nanorods is attributed to the increased reactivity of the side facets, due to less surface passivation of cetyltrimethylammonium bromide. The similar synthetic strategy has also been demonstrated to be successful for the Pd-tipped Au nanorods that have not been reported before, indicating the great potential of this selective etching. The Ag-tipped Au nanorods are examined as a catalyst for the reduction of p-nitrophenol at room temperature. The Ag-tipped Au nanorods exhibit a higher catalytic activity than Au nanorods and core-shell Au@Ag nanorods, which could be attributed to the electronic effect and the unique structure in the Ag-tipped Au nanorods.

Fast-response and high-sensitivity deep-ultraviolet (DUV) photodetectors with detection wavelength shorter than 320 nm are in high demand due to their potential applications in diverse fields. However, the fabrication processes of DUV detectors based on traditional semiconductor thin films are complicated and costly. Here we report a high-performance DUV photodetector based on graphene quantum dots (GQDs) fabricated via a facile solution process. The devices are capable of detecting DUV light with wavelength as short as 254 nm. With the aid of an asymmetric electrode structure, the device performance could be significantly improved. An on/off ratio of ∼6000 under 254 nm illumination at a relatively weak light intensity of 42 μW cm(-2) is achieved. The devices also exhibit excellent stability and reproducibility with a fast response speed. Given the solution-processing capability of the devices and extraordinary properties of GQDs, the use of GQDs will open up unique opportunities for future high-performance, low-cost DUV photodetectors.