Vertical heterostructures based on two-dimensional(2D)materials have attracted widespread interest for their numerous applications in electronic and optoelectronic devices.Herein,we report the direct construct!on of a...Vertical heterostructures based on two-dimensional(2D)materials have attracted widespread interest for their numerous applications in electronic and optoelectronic devices.Herein,we report the direct construct!on of an abnormal graphene/ReSe2 stack on Au foils by a two-step chemical vapor deposition(CVD)strategy.During the second growth stage,mono layer ReSe2 is found to prefere ntially evolve at the irUerface between the first-grown graphene layer and the Au substrate.The unusual stacking behavior is unraveled by in-situ"cutting open"the upper graphene from the defects to expose the lower ReSe2 using scanning tunneling microscopy(STM).From combination of these results with density functional theory calculations,the domain boundaries and edge sites of graphene are proposed to be adsorption sites for Re and Se precursors,further facilitating the growth of ReSe2 at the van der Waals gap of graphene/Au.This work hereby offers an intriguing strategy for obtaining vertical 2D heterostructures featured with an ultra-clean interface and a designed stacking geometry.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDCs)have emerged as perfect platforms for developing applications in nano-electronics,catalysis,energy storage and environmental-related fields due to their superi...Two-dimensional(2D)transition metal dichalcogenides(TMDCs)have emerged as perfect platforms for developing applications in nano-electronics,catalysis,energy storage and environmental-related fields due to their superior properties.However,the low-cost,batch production of high-quality 2D TMDCs remains a huge challenge with the existing synthetic strategies.Herein,we present a scalable chemical vapor deposition(CVD)approach for the batch production of high-quality MoS_(2) nanosheet powders,by using naturally abundant,water-soluble and recyclable NaCl crystal powders as templates.The high-quality MoS_(2) nanosheets powders are achieved by a facile water dissolution-filtration process,by virtue of the excellent dispersibility of the as-grown products in water.The internal mechanism for the scalable synthesis strategy is explored.The applications of the MoS_(2) nanosheets powders are also demonstrated as catalysts or adsorbents in hydrogen evolution reaction(HER)and organic dyes adsorption,respectively.This work should hereby pave ways for the mass production and application of powdery TMDCs in energetic and environmental related fields.展开更多
Owing to its anisotropic optical and electrical properties,rhenium diselenide(ReSe2)has garnered considerable attention recently as a candidate material for polarization-sensitive photodetectors.However,the direct and...Owing to its anisotropic optical and electrical properties,rhenium diselenide(ReSe2)has garnered considerable attention recently as a candidate material for polarization-sensitive photodetectors.However,the direct and controllable synthesis of large-sized ReSe2 with a uniform thickness is still a great challenge.Herein,we have refined the synthesis method to obtain uniform monolayer ReSe2 flakes with a size of up to^106μm on sapphire via an ambient-pressure chemical vapor deposition technique using Na promoter from sodium chloride.Interestingly,optical pump-probe spectroscopy revealed a fast switching from saturable absorption(SA)to absorption enhancement(AE)in subpicosecond time scale,followed by a slower decay induced by exciton recombination.Furthermore,both AE and SA signals exhibited clear angular dependence with a periodicity of 180°,which reflected the dichroism in nonlinear absorption dynamics.In addition,the photocarrier dynamics including free-carrier transport and subpicosecond relaxation due to exciton formation or surface trapping was probed using time resolved terahertz spectroscopy.We believe that our study serves as a reference for atomically controlled synthesis of large-sized ReSe2 and provides useful insights on its optoelectronic properties for novel device applications.展开更多
Controlled synthesis of structurally anisotropic rhenium diselenide (ReSe2) with macroscopically uniform and strictly monolayer thickness as well as tunable domain shape/size is of great interest for electronics-, o...Controlled synthesis of structurally anisotropic rhenium diselenide (ReSe2) with macroscopically uniform and strictly monolayer thickness as well as tunable domain shape/size is of great interest for electronics-, optoelectronics-, and electrocatalysis-related applications. Herein, we describe the controlled synthesis of uniform monolayer ReSe2 flakes with variable morphology (sunflower- or truncated-triangle-shaped) on SiO2/Si substrates using different ambient-pressure chemical vapor deposition (CVD) setups. The prepared polycrystalline ReSe2 flakes were transferred intact onto Au foil electrodes and tested for activity in the hydrogen evolution reaction (HER). Interestingly, compared to the compact truncated-triangle-shaped ReSe2 flakes, their edge-abundant sunflower-shaped counterparts exhibited superior electrocatalytic HER activity, featuring a relatively low Tafel slope of - 76 mV/dec and an exchange current density of 10.5 μA/cm2. Thus, our work demonstrates that CVD-grown ReSe2 is a promising two- dimensional anisotropic material for applications in the electrocatalytic HER.展开更多
The emerging two-dimensional(2D)platinum disulfide(PtS_(2))has driven increasing attentions due to its high electron mobility,good air-stability,and strong interlayer interaction which leads to a widely tunable electr...The emerging two-dimensional(2D)platinum disulfide(PtS_(2))has driven increasing attentions due to its high electron mobility,good air-stability,and strong interlayer interaction which leads to a widely tunable electronic structure.However,a detailed study on its covalent-like layer-dependent properties remains infant.Herein,we demonstrate the successful production of ultrathin 1T-PtS_(2) ribbons with thickness centralized almost at monolayer 1L-4L and large domain size up to 210 μm on Au foils using chemical vapor deposition(CVD)technique,which enables macro-and microscopic study of its extraordinary layer-dependent features with precise control of the number of layers.Using electron energy loss spectroscopy(EELS)and optical pump-probe spectroscopy(OPPS),we reveal that both the electron and ultrafast optical absorption signals of the as-grown 2D PtS_(2) show strong nonlinear layer-dependent responses which manifest discriminated transition in 1L-4L PtS_(2) ribbons.The layer-dependent nonlinear response of 2D PtS_(2) can be well interpreted in the frame of calculated electron and phonon structures.These achievements offer a platform for successfully fabricating large-sized ultrathin 2D PtS_(2) and facilitating our knowledge about its electronic and optoelectronic properties.展开更多
基金the National Natural Science Foundation of China(Nos.51472008,51861135201,51290272,61774003,51502007,and 51672007)the National Key Research and Development Program of China(Nos.2016YFA0200103,2017YFA0205700,and 2017YFA0304600)+1 种基金the Open Research Fund Program of the State Key Laboratory of Low-Dimensional Quantum Physics(Nos.KF201601 and KF201604)"2011 Program”Peking-Tsinghua-IOP Collaborative Innovation Center of Quantum Matter.
文摘Vertical heterostructures based on two-dimensional(2D)materials have attracted widespread interest for their numerous applications in electronic and optoelectronic devices.Herein,we report the direct construct!on of an abnormal graphene/ReSe2 stack on Au foils by a two-step chemical vapor deposition(CVD)strategy.During the second growth stage,mono layer ReSe2 is found to prefere ntially evolve at the irUerface between the first-grown graphene layer and the Au substrate.The unusual stacking behavior is unraveled by in-situ"cutting open"the upper graphene from the defects to expose the lower ReSe2 using scanning tunneling microscopy(STM).From combination of these results with density functional theory calculations,the domain boundaries and edge sites of graphene are proposed to be adsorption sites for Re and Se precursors,further facilitating the growth of ReSe2 at the van der Waals gap of graphene/Au.This work hereby offers an intriguing strategy for obtaining vertical 2D heterostructures featured with an ultra-clean interface and a designed stacking geometry.
基金supported by the National Key Research and Development Program of China(No.2018YFA0703700)the National Natural Science Foundation of China(Nos.51991340,51991344,and 51861135201)the Beijing Natural Science Foundation(No.2192021).
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDCs)have emerged as perfect platforms for developing applications in nano-electronics,catalysis,energy storage and environmental-related fields due to their superior properties.However,the low-cost,batch production of high-quality 2D TMDCs remains a huge challenge with the existing synthetic strategies.Herein,we present a scalable chemical vapor deposition(CVD)approach for the batch production of high-quality MoS_(2) nanosheet powders,by using naturally abundant,water-soluble and recyclable NaCl crystal powders as templates.The high-quality MoS_(2) nanosheets powders are achieved by a facile water dissolution-filtration process,by virtue of the excellent dispersibility of the as-grown products in water.The internal mechanism for the scalable synthesis strategy is explored.The applications of the MoS_(2) nanosheets powders are also demonstrated as catalysts or adsorbents in hydrogen evolution reaction(HER)and organic dyes adsorption,respectively.This work should hereby pave ways for the mass production and application of powdery TMDCs in energetic and environmental related fields.
基金The work was supported by the National Key Research and Development Program of China(Nos.2018YFA0703700,2017YFA0304600,and 2017YFA0205700)the National Natural Science Foundation of China(Nos.51861135201,21473001,11774354,11674329,and 51727806)+4 种基金Beijing Natural Science Foundation(No.2192021)the Project funded by China Postdoctoral Science Foundation(No.2018M640023)Chinese Academy of Science(No.YZJJ201705)Open Research Fund Program of the State Key Laboratory of Low-dimensional Quantum Physics(No.KF201907)Start-up Funding of Peking University.
文摘Owing to its anisotropic optical and electrical properties,rhenium diselenide(ReSe2)has garnered considerable attention recently as a candidate material for polarization-sensitive photodetectors.However,the direct and controllable synthesis of large-sized ReSe2 with a uniform thickness is still a great challenge.Herein,we have refined the synthesis method to obtain uniform monolayer ReSe2 flakes with a size of up to^106μm on sapphire via an ambient-pressure chemical vapor deposition technique using Na promoter from sodium chloride.Interestingly,optical pump-probe spectroscopy revealed a fast switching from saturable absorption(SA)to absorption enhancement(AE)in subpicosecond time scale,followed by a slower decay induced by exciton recombination.Furthermore,both AE and SA signals exhibited clear angular dependence with a periodicity of 180°,which reflected the dichroism in nonlinear absorption dynamics.In addition,the photocarrier dynamics including free-carrier transport and subpicosecond relaxation due to exciton formation or surface trapping was probed using time resolved terahertz spectroscopy.We believe that our study serves as a reference for atomically controlled synthesis of large-sized ReSe2 and provides useful insights on its optoelectronic properties for novel device applications.
基金The work was supported by the National Natural Science Foundation of China (Nos. 51290272, 51472008, 21573004, 51522212, 51421002, 51672154, 51372130, and 51672307), the National Key Technologies Research and Development Program of China (No. 2016YFA0200103), the Open Research Fund Program of the State Key Laboratory of Low-Dimensional Quantum Physics (No. KF201601), the National Program on Key Basic Research Project (No. 2014CB921002), the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB07030200), the Key Research Program of Frontier Sciences, CAS (No. QYZDB-SSW-JSC035), and the MoST (2016YFA0200200).
文摘Controlled synthesis of structurally anisotropic rhenium diselenide (ReSe2) with macroscopically uniform and strictly monolayer thickness as well as tunable domain shape/size is of great interest for electronics-, optoelectronics-, and electrocatalysis-related applications. Herein, we describe the controlled synthesis of uniform monolayer ReSe2 flakes with variable morphology (sunflower- or truncated-triangle-shaped) on SiO2/Si substrates using different ambient-pressure chemical vapor deposition (CVD) setups. The prepared polycrystalline ReSe2 flakes were transferred intact onto Au foil electrodes and tested for activity in the hydrogen evolution reaction (HER). Interestingly, compared to the compact truncated-triangle-shaped ReSe2 flakes, their edge-abundant sunflower-shaped counterparts exhibited superior electrocatalytic HER activity, featuring a relatively low Tafel slope of - 76 mV/dec and an exchange current density of 10.5 μA/cm2. Thus, our work demonstrates that CVD-grown ReSe2 is a promising two- dimensional anisotropic material for applications in the electrocatalytic HER.
基金The work was supported by the National Natural Science Foundation of China(Nos.51991344,51991340,11774354,51727806,61988102,11974156,12174398,and 12104206)Guangdong International Science Collaboration Project(No.2019A050510001)+2 种基金Guangdong Innovative and Entrepreneurial Research Team Program(No.2019ZT08C044)Shenzhen Science and Technology Program(Nos.KQTD20190929173815000 and 20200925161102001)the Science,Technology and Innovation Commission of Shenzhen Municipality(No.ZDSYS20190902092905285)。
文摘The emerging two-dimensional(2D)platinum disulfide(PtS_(2))has driven increasing attentions due to its high electron mobility,good air-stability,and strong interlayer interaction which leads to a widely tunable electronic structure.However,a detailed study on its covalent-like layer-dependent properties remains infant.Herein,we demonstrate the successful production of ultrathin 1T-PtS_(2) ribbons with thickness centralized almost at monolayer 1L-4L and large domain size up to 210 μm on Au foils using chemical vapor deposition(CVD)technique,which enables macro-and microscopic study of its extraordinary layer-dependent features with precise control of the number of layers.Using electron energy loss spectroscopy(EELS)and optical pump-probe spectroscopy(OPPS),we reveal that both the electron and ultrafast optical absorption signals of the as-grown 2D PtS_(2) show strong nonlinear layer-dependent responses which manifest discriminated transition in 1L-4L PtS_(2) ribbons.The layer-dependent nonlinear response of 2D PtS_(2) can be well interpreted in the frame of calculated electron and phonon structures.These achievements offer a platform for successfully fabricating large-sized ultrathin 2D PtS_(2) and facilitating our knowledge about its electronic and optoelectronic properties.