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A four-state fluorescent molecular switch
摘要： Cross-coupling reactions are among the most powerful C–C and C–X bond forming tools in organic chemistry. Traditionally, cross-coupling methods rely on the use of aryl halides or pseudohalides as electrophiles. In the past three years, decarbonylative cross-couplings of amides have emerged as an attractive method for the construction of a wide variety of carbon–carbon and carbon–heteroatom bonds, allowing for the synthetically-valuable functional group inter-conversion of the amide bond. These previously elusive reactions hinge upon selective activation of the N–C(O) acyl amide bond, followed by CO extrusion, in a formal double N–C/C–C bond activation, to generate a versatile aryl–metal intermediate as an attractive alternative to traditional cross-couplings of aryl halides and pseudohalides. In this perspective review, we present recent advances and key developments in the field of decarbonylative cross-coupling reactions of amides as well as discuss future challenges and potential applications for this exciting field.
关键词： amides,transition-metal catalysis,C–C bond formation,decarbonylative cross-coupling,C–X bond formation
更新于2025-09-19 17:15:36
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Synthesis and Characterization of a Rare Transition-Metal Oxothiostannate and Investigation of Its Photocatalytic Properties
摘要： The new transition-metal oxothiostannate [Ni(cyclen)(H2O)2]4[Sn10S20O4]·～13H2O (1) was prepared under hydrothermal conditions using Na4SnS4·14H2O as the precursor in the presence of [Ni(cyclen)(H2O)2](ClO4)2·H2O. Compound 1 comprises the [Sn10S20O4]8? anion constructed by the T3-type supertetrahedron [Sn10S20] and the [Sn10O4] anti-T2 cluster. Channels host the H2O molecules, and the sample can be reversibly dehydrated and rehydrated without significantly affecting the crystallinity of the material. 119Sn NMR spectroscopy of an aqueous solution of Na4SnS4·14H2O evidences that between 25 and 120 °C only [SnS4]4? and [Sn2S6]4? anions are present. In further experiments, hints were found that the formation of the tin oxosulfide ions depends on the Ni2+-centered complexes. Compound 1 exhibits promising photocatalytic properties for the visible-light-driven hydrogen evolution reaction, with 18.7 mmol·g?1 H2 being evolved after 3 h.
关键词： photocatalytic hydrogen evolution,oxothiostannate,NMR spectroscopy,hydrothermal synthesis,transition-metal complex
更新于2025-09-19 17:15:36
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Electronic and optical characterization of 2D Ti<sub>2</sub>C and Nb<sub>2</sub>C (MXene) thin films
摘要： Two-dimensional (2D) transition metal carbides and/or nitrides (MXenes) are emerging as a new class of 2D materials, with extensive opportunities for property tailoring due to the numerous possibilities for varying chemistries and surface terminations. Here, Ti2AlC and Nb2AlC MAX phase epitaxial thin films were deposited on sapphire substrates by physical vapor deposition. The films were then etched in LiF/HCl solutions, yielding Li-intercalated, 2D Ti2CTz and Nb2CTz films, whose terminations, transport and optical properties were characterized. The former exhibits metallic conductivity, with weak localization below 50 K. In contrast, the Nb-based film exhibits an increase in resistivity with decreasing temperature from RT down to 40 K consistent with variable range hopping transport. The optical properties of both films were determined from spectroscopic ellipsometry in the 0.75 to 3.50 eV range. The results for Ti2AlTz films confirm the metallic behavior. In contrast, no evidence of metallic behavior is observed for the Nb2CTz film. The present work therefore demonstrates that one fruitful approach to alter the electronic and optical properties of MXenes is to change the nature of the transition metal.
关键词： transition metal carbide,thin films,MXene,transport properties
更新于2025-09-19 17:15:36
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Thickness-controlled synthesis of CoX2 (X = S, Se, Te) single crystalline 2D layers with linear magnetoresistance and high conductivity.
摘要： Two-dimensional (2D) materials especially transition metal dichalcogenides (TMDs) have drawn intensive interests owing to their plentiful properties. Some TMDs with magnetic elements (Fe, Co, Ni, etc.) are reported to be magnetic theoretically and experimentally, which undoubtedly provide a promising platform to design functional devices and study physical mechanisms. Nevertheless, plenty of the theoretical TMDs remain unrealized experimentally. In addition, the governable synthesis of these kinds of TMDs with desired thickness and high crystallinity poses a tricky challenge. Here, we report a controlled preparation of CoX2 (X = S, Se, Te) nanosheets through chemical vapor deposition (CVD). The thickness, lateral scale and shape of the crystals show great dependence with temperature and the thickness can be controlled from monolayer to tens of nanometers. Magneto-transport characterization and Density Function Theory (DFT) simulation indicate CoSe2 and CoTe2 are metallic. Besides, unsaturated and linear magnetoresistance have been observed even up to 9 Tesla. The conductivity of CoSe2 and CoTe2 can reach 5 × 106 and 1.8 × 106 S/m respectively, which is pretty high and even comparable with silver. These cobalt-based TMDs show great potential to work as 2D conductors and also provide a promising platform for investigating their magnetic properties.
关键词： Transition metal dichalcogenides,Magnetoresistance,Conductivity,Two-dimensional materials,Chemical vapor deposition
更新于2025-09-19 17:13:59
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Photocontrolled synthesis of na??type conjugated polymers
摘要： Current approaches to synthesize π-conjugated polymers (CPs) are dominated by thermally driven, transition metal-mediated reactions. Herein we show that electron-deficient Grignard monomers readily polymerize under visible light irradiation at room temperature in the absence of a catalyst. The product distribution can be tuned by the wavelength of irradiation based on the absorption of the polymer. Conversion studies are consistent with an uncontrolled chain-growth process; correspondingly, chain extension produces all-conjugated n-type block copolymers. Preliminary results demonstrate that the polymerization can be expanded to donor-acceptor alternating copolymers. We anticipate that this method can serve as a platform to access new architectures of n-type CPs without the need for transition metal catalysis.
关键词： photopolymerization,transition-metal-free,conjugated polymer
更新于2025-09-19 17:13:59
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Enhanced Absorption in MoS <sub/>2</sub> /Hg <sub/>0.33</sub> Cd <sub/>0.66</sub> Te Heterostructure for Application in Solar Cell Absorbers
摘要： The heterostructure of mercury cadmium telluride (Hg0.33Cd0.66Te) and monolayer MoS2 with Van der Waals (VdW) interaction is suggested for tuning the optical absorption in visible region. The calculations are performed using density functional theory (DFT). From the results, it is found that for molybdenum disulfide (MoS2) absorption is high in the ～390–430 nm range of visible region and for mercury cadmium telluride (Hg0.33Cd0.66Te) absorption is high in the ～310–350 nm. However, absorption in the MoS2/Hg0.33Cd0.66Te heterostructure increases with the wavelength and also shifts towards the red region of the visible spectrum, resulting into a well known red-shift phenomenon. Moreover, higher absorption is seen (entirely in visible region) in the heterostructure in the desired visible region range (λ ～640–710 nm) of the spectrum required for application in optoelectronic devices. The heterostructure results into semi-metallic or negligible indirect bandgap creation in contrast to direct bandgap observed in individual MoS2 and Hg0.33Cd0.66Te structures. The heterostructure can find application in Schottky barrier solar cell absorbers.
关键词： Optoelectronics,solar cells,transition metal dichalcogenides,absorption coefficient,refractive index
更新于2025-09-19 17:13:59
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Waveguide-integrated van der Waals heterostructure photodetector at telecom wavelengths with high speed and high responsivity
摘要： Intensive efforts have been devoted to the exploration of new optoelectronic devices based on two-dimensional transition-metal dichalcogenides (TMDCs) owing to their strong light–matter interaction and distinctive material properties. In particular, photodetectors featuring both high-speed and high-responsivity performance are of great interest for a vast number of applications such as high-data-rate interconnects operated at standardized telecom wavelengths. Yet, the intrinsically small carrier mobilities of TMDCs become a bottleneck for high-speed application use. Here, we present high-performance vertical van der Waals heterostructure-based photodetectors integrated on a silicon photonics platform. Our vertical MoTe2–graphene heterostructure design minimizes the carrier transit path length in TMDCs and enables a record-high measured bandwidth of at least 24 GHz under a moderate bias voltage of –3 V. Applying a higher bias or employing thinner MoTe2 flakes boosts the bandwidth even to 50 GHz. Simultaneously, our device reaches a high external responsivity of 0.2 A W–1 for incident light at 1,300 nm, benefiting from the integrated waveguide design. Our studies shed light on performance trade-offs and present design guidelines for fast and efficient devices. The combination of two-dimensional heterostructures and integrated guided-wave nano photonics defines an attractive platform to realize high-performance optoelectronic devices, such as photodetectors, light-emitting devices and electro-optic modulators.
关键词： transition-metal dichalcogenides,photodetectors,silicon photonics,van der Waals heterostructures,two-dimensional materials
更新于2025-09-19 17:13:59
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Recent progress in ultrafast lasers based on 2D materials as a saturable absorber
摘要： Two-dimensional (2D) materials are crystals with one to a few layers of atoms and are being used in many fields such as optical modulator, photodetector, optical switch, and ultrafast lasers. Their exceptional optoelectronic and nonlinear optical properties make them as a suitable saturable absorber for laser cavities. This review focuses on the recent progress in ultrafast laser use 2D materials as a saturable absorber. 2D materials traditionally include graphene, topological insulators, transition metal dichalcogenides, as well as new materials such as black phosphorus, bismuthene, antimonene, and MXene. Material characteristics, fabrication techniques, and nonlinear properties are also introduced. Finally, future perspectives of ultrafast lasers based on 2D materials are also addressed.
关键词： saturable absorber,MXene,antimonene,bismuthene,graphene,ultrafast lasers,transition metal dichalcogenides,black phosphorus,2D materials,topological insulators
更新于2025-09-19 17:13:59
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Colour centre controlled formation of stable sub-nanometer transition metal clusters on TiO2 nanosheet for high efficient H2 production
摘要： The transition elements (Fe, Co, Ni) are important substitutes for noble metals as the co-catalysts in hydrogen evolution reaction. Enhancing the atom utilization efficiency is highly desirable, but preparation and preservation of the transition metal catalysts with the size downscaling to sub-nanometer are challenging. In this work, Fe, Co and Ni clusters with subnano size as co-catalysts are synthesized by controllable growth on 2D ultrathin TiO2(B) nanosheets for hydrogen evolution using a photo deposition method. The ultra-small Fe, Co, and Ni co-catalysts on the TiO2(B) nanosheets exhibit remarkably enhanced photo activities, compared to that with the best Pt loading. It is found that the oxygen bridge vacancies act as the colour centres locating at the position adjacent to the O1-Ti1 sites on the TiO2(B) (001) surface. The photo-colouration and photo-bleaching have significantly impact on the nucleation and growth of the metallic clusters. The high density and uniform dispersion of the sub-nano-sized transition metal clusters benefits for the photo reduction under light irradiation, as well as efficient carrier separation, leading to a great improvement of the photo activity.
关键词： TiO2(B),transition metal loading,photocatalysis,water splitting,sub-nanometer
更新于2025-09-19 17:13:59
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Thickness dependence of solar cell efficiency in transition metal dichalcogenides MX2 (M: Mo, W; X: S, Se, Te)
摘要： Bulk transition metal dichalcogenides are indirect gap semiconductors with optical gaps in the range of 0.7–1.6 eV, which makes them suitable for solar cell applications. In this work, we study the electronic structure, optical properties, and the thickness dependence of the solar cell efficiencies of MX2 (M: Mo, W; X: S, Se, Te) with density functional theory and GW t BSE. Through this analysis, we find a change in solar cell efficiency trends at slab thicknesses of 3 μm. For thin films solar cells (thicknesses smaller than 3 μm), the tellurides present the highest efficiencies (about 20% for a 100 nm thick slab). In contrast, for thicknesses greater than 3 μm, our results indicate that a maximum solar cell efficiency can be achieved in WS2. For instance, a 100 μm slab of WS2 presents a solar cell efficiency of 36.3%, making this material a promising candidate for solar cell applications.
关键词： Thin film,First-principles,DFT,Solar cell,Transition metal dichalcogenides,GWtBSE
更新于2025-09-19 17:13:59