Exploring high efficiency S-scheme heterojunction photocatalysts with strong redox ability for removing volatile organic compounds from the air is of great interest and importance.However,how to predict and regulate t...Exploring high efficiency S-scheme heterojunction photocatalysts with strong redox ability for removing volatile organic compounds from the air is of great interest and importance.However,how to predict and regulate the transport of photogenerated carriers in heterojunctions is a great challenge.Here,density functional theory calculations were first used to successfully predict the formation of a CdS quantum dots/InVO_(4)atomic-layer(110)/(110)facet S-scheme heterojunction.Subsequently,a CdS quantum dots/InVO_(4)atomic-layer was synthesized by in-situ loading of CdS quantum dots with(110)facets onto the(110)facets of InVO_(4)atomic-layer.As a result of the deliberately constructed built-in electric field between the adjoining facets,we obtain a remarkably enhanced photocatalytic degradation rate for ethylene.This rate is 13.8 times that of pure CdS and 13.2 times that of pure InVO_(4).In-situ irradiated X-ray photoelectron spectroscopy,photoluminescence and time-resolved photoluminescence measurements were carried out.These experiments validate that the built-in electric field enhanced the dissociation of photoexcited excitons and the separation of free charge carriers,and results in the formation of S-scheme charge transfer pathways.The reaction mechanism of the photocatalytic C_(2)H_(4)oxidation is investigated by in-situ electron paramagnetic resonance.This work provides a mechanistic insight into the construction and optimization of semiconductor heterojunction photocatalysts for application to environmental remediation.展开更多
Atomic-layer MoS_2 ultrathin films are synthesized using a hot filament chemical vapor deposition method. A combination of atomic force microscopy（AFM）, x-ray diffraction（XRD）, high-resolution transition electron ...Atomic-layer MoS_2 ultrathin films are synthesized using a hot filament chemical vapor deposition method. A combination of atomic force microscopy（AFM）, x-ray diffraction（XRD）, high-resolution transition electron microscopy（HRTEM）, photoluminescence（PL）, and x-ray photoelectron spectroscopy（XPS） characterization methods is applied to investigate the crystal structures, valence states, and compositions of the ultrathin film areas. The nucleation particles show irregular morphology, while for a larger size somewhere, the films are granular and the grains have a triangle shape. The films grow in a preferred orientation（002）. The HRTEM images present the graphene-like structure of stacked layers with low density of stacking fault, and the interlayer distance of plane is measured to be about 0.63 nm. It shows a clear quasihoneycomb-like structure and 6-fold coordination symmetry. Room-temperature PL spectra for the atomic layer MoS_2 under the condition of right and left circular light show that for both cases, the A1 and B1 direct excitonic transitions can be observed. In the meantime, valley polarization resolved PL spectra are obtained. XPS measurements provide high-purity samples aside from some contaminations from the air, and confirm the presence of pure MoS_2. The stoichiometric mole ratio of S/Mo is about 2.0–2.1, suggesting that sulfur is abundant rather than deficient in the atomic layer MoS_2 under our experimental conditions.展开更多
Accumulation-type GaN metal-oxide-semiconductor field-effect transistors （MOSFETs） with atomic-layer- deposited A1203 gate dielectrics are fabricated. The device, with atomic-layer-deposited A1203 as the gate dielec...Accumulation-type GaN metal-oxide-semiconductor field-effect transistors （MOSFETs） with atomic-layer- deposited A1203 gate dielectrics are fabricated. The device, with atomic-layer-deposited A1203 as the gate dielectric, presents a drain current of 260 mA/mm and a broad maximum transconductance of 34 mS/mm, which are better than those reported previously with Al203 as the gate dielectric. Furthermore, the device shows negligible current collapse in a wide range of bias voltages, owing to the effective passivation of the GaN surface by the A1203 film. The gate drain breakdown voltage is found to be about 59.5 V, and in addition the channel mobility of the n-GaN layer is about 380 cm^2/Vs, which is consistent with the Hall result, and it is not degraded by atomic-layer-deposition A1203 growth and device fabrication.展开更多
Control of surface structure at the atomic level can effectively tune catalytic properties of nanomaterials.Tuning surface strain is an effective strategy for enhancing catalytic activity;however,the correlation studi...Control of surface structure at the atomic level can effectively tune catalytic properties of nanomaterials.Tuning surface strain is an effective strategy for enhancing catalytic activity;however,the correlation studies between the surface strain with catalytic performance are scant because such mechanistic studies require the precise control of surface strain on catalysts.In this work,a simple strategy of precisely tuning compressive surface strain of atomic-layer Cu2O on Cu@Ag (AL-Cu2O/Cu@Ag) nanoparticles (NPs) is demonstrated.The AL-Cu2O is synthesized by structure evolution of Cu@Ag core-shell nanoparticles,and the precise thickness-control of AL-Cu2O is achieved by tuning the molar ratio of Cu/Ag of the starting material.Aberration-corrected high-resolution transmission electron microscopy (AC-HRTEM) and EELS elemental mapping characterization showed that the compressive surface strain of AL-Cu2O along the [111] and [200] directions can be precisely tuned from 6.5% to 1.6% and 6.6% to 4.7%,respectively,by changing the number of AL-Cu2O layer from 3 to 6.The as-prepared AL-Cu2O/Cu@Ag NPs exhibited excellent catalytic property in the synthesis of azobenzene from aniline,in which the strained 4-layers Cu2O (4.5% along the [111] direction,6.1% along the [200] direction) exhibits the best catalytic performance.This work may be beneficial for the design and surface engineering of catalysts toward specific applications.展开更多
Er2O3 thin films are grown on oxidized Si （111） substrates by molecular beam epitaxy. The sample grown under optimized condition is characterized in its microstructure, surface morphology and thickness using grazing...Er2O3 thin films are grown on oxidized Si （111） substrates by molecular beam epitaxy. The sample grown under optimized condition is characterized in its microstructure, surface morphology and thickness using grazing incidence x-ray diffraction （GIXRD）, atomic force morphology and x-ray reflectivity. GIXRD measurements reveal that the Er2O3 thin film is a mosaic of single-crystal domains. The interplanar spacing d in-plane residual strain tensor ell and the strain relaxation degree ε are calculated. The Poisson ratio μ obtained by conventional x-ray diffraction is in good agreement with that of the bulk Er2O3. In-plane strains in three sets of planes, i.e. （440）, （404）, and （044）, are isotropic.展开更多
In our experiment, an atomic layer MoS2structure grown on SiO2/Si substrates is used in transport test. The voltage U14,23 oscillates and the corresponding period varies with applied current. The largest period appear...In our experiment, an atomic layer MoS2structure grown on SiO2/Si substrates is used in transport test. The voltage U14,23 oscillates and the corresponding period varies with applied current. The largest period appears at 45 μA. The oscillation periods are different when samples are under laser radiation or in darkness. We discover that under the laser irradiation, the oscillation period occurs at lower current than in the darkness case. Meanwhile, the drift velocity is estimated at ~10~7 cm/s. Besides, by studying the envelope of U14,23 versus applied current, we see a beating phenomenon at a certain current value. The beating period in darkness is larger than under laser irradiation. The difference between beating periods reveals the energy difference of electrons. Similar results are obtained by using different laser power densities and different light sources. The possible mechanism behind the oscillation period is discussed.展开更多
The nonlinear Hall effect(NLHE)has attracted extensive attention due to its complex physical origins and rectification characteristics with time-reversal symmetry.However,the special symmetry requirements have restric...The nonlinear Hall effect(NLHE)has attracted extensive attention due to its complex physical origins and rectification characteristics with time-reversal symmetry.However,the special symmetry requirements have restricted the research and application of NLHE.Here we have developed an in-situ on-device electrochemical intercalation method to fabricate cetyltrimethylammonium cation(CTA^(+))intercalated MoS_(2) device.Structural characterization demonstrates that owing to the intercalation of CTA+,the atomic structure within the layers remains unchanged,but the layer distance expands from 0.61 nm to 1.06 nm,distinguish with the previous research.Due to the substantial injection of electrons by the intercalation process,the transport behavior of MoS_(2) transforms from semi-metallic to metallic.By breaking of inversion symmetry introduced by the intercalation of CTA^(+),NLHE is induced.In the measurement of temperature-dependent NLHE,not only the main mechanism of skew scattering is confirmed by the nonlinear susceptibility analysis,but also a significant NLHE with the second-harmonic nonlinear Hall coefficient can be still observed under room temperature of 300 K.Our work expands the candidates of room-temperature NLHE materials and provides a new perspective for investigating the NLHE and symmetry engineering in two-dimensional materials.展开更多
基金financially supported by the National Natural Science Foundation of China(Grant No.21902046,21801071,12174092,U21A20500)Overseas Expertise Introduction Center for Discipline Innovation(D18025)+3 种基金the Natural Science Foundation of Hubei Provincial(Grant No.2018CFB171)Wuhan Science and Technology Bureau(2020010601012163)Science and Technology Research Project of Hubei Provincial Department of Education(No.D20221001)the open foundation of the State Key Laboratory of Structural Chemistry,Fujian Institute of Research on the Structure of Matter,Chinese Academy of Sciences
文摘Exploring high efficiency S-scheme heterojunction photocatalysts with strong redox ability for removing volatile organic compounds from the air is of great interest and importance.However,how to predict and regulate the transport of photogenerated carriers in heterojunctions is a great challenge.Here,density functional theory calculations were first used to successfully predict the formation of a CdS quantum dots/InVO_(4)atomic-layer(110)/(110)facet S-scheme heterojunction.Subsequently,a CdS quantum dots/InVO_(4)atomic-layer was synthesized by in-situ loading of CdS quantum dots with(110)facets onto the(110)facets of InVO_(4)atomic-layer.As a result of the deliberately constructed built-in electric field between the adjoining facets,we obtain a remarkably enhanced photocatalytic degradation rate for ethylene.This rate is 13.8 times that of pure CdS and 13.2 times that of pure InVO_(4).In-situ irradiated X-ray photoelectron spectroscopy,photoluminescence and time-resolved photoluminescence measurements were carried out.These experiments validate that the built-in electric field enhanced the dissociation of photoexcited excitons and the separation of free charge carriers,and results in the formation of S-scheme charge transfer pathways.The reaction mechanism of the photocatalytic C_(2)H_(4)oxidation is investigated by in-situ electron paramagnetic resonance.This work provides a mechanistic insight into the construction and optimization of semiconductor heterojunction photocatalysts for application to environmental remediation.
基金Project supported by the Natural Science Foundation of Zhejiang Province,China(Grant Nos.LY16F040003 and LY16A040007)the National Natural Science Foundation of China(Grant Nos.51401069 and 11574067)
文摘Atomic-layer MoS_2 ultrathin films are synthesized using a hot filament chemical vapor deposition method. A combination of atomic force microscopy（AFM）, x-ray diffraction（XRD）, high-resolution transition electron microscopy（HRTEM）, photoluminescence（PL）, and x-ray photoelectron spectroscopy（XPS） characterization methods is applied to investigate the crystal structures, valence states, and compositions of the ultrathin film areas. The nucleation particles show irregular morphology, while for a larger size somewhere, the films are granular and the grains have a triangle shape. The films grow in a preferred orientation（002）. The HRTEM images present the graphene-like structure of stacked layers with low density of stacking fault, and the interlayer distance of plane is measured to be about 0.63 nm. It shows a clear quasihoneycomb-like structure and 6-fold coordination symmetry. Room-temperature PL spectra for the atomic layer MoS_2 under the condition of right and left circular light show that for both cases, the A1 and B1 direct excitonic transitions can be observed. In the meantime, valley polarization resolved PL spectra are obtained. XPS measurements provide high-purity samples aside from some contaminations from the air, and confirm the presence of pure MoS_2. The stoichiometric mole ratio of S/Mo is about 2.0–2.1, suggesting that sulfur is abundant rather than deficient in the atomic layer MoS_2 under our experimental conditions.
文摘Accumulation-type GaN metal-oxide-semiconductor field-effect transistors （MOSFETs） with atomic-layer- deposited A1203 gate dielectrics are fabricated. The device, with atomic-layer-deposited A1203 as the gate dielectric, presents a drain current of 260 mA/mm and a broad maximum transconductance of 34 mS/mm, which are better than those reported previously with Al203 as the gate dielectric. Furthermore, the device shows negligible current collapse in a wide range of bias voltages, owing to the effective passivation of the GaN surface by the A1203 film. The gate drain breakdown voltage is found to be about 59.5 V, and in addition the channel mobility of the n-GaN layer is about 380 cm^2/Vs, which is consistent with the Hall result, and it is not degraded by atomic-layer-deposition A1203 growth and device fabrication.
基金the National Natural Science Foundation of China (Nos.51631001,21643003,51872030,51702016,and 51501010)Fundamental Research Funds for the Central Universities, Beijing Institute of Technology Research Fund Program for Young Scholars and ZDKT18-01 from State Key Laboratory of Explosion Science and Technology (Beijing Institute of Technology).
文摘Control of surface structure at the atomic level can effectively tune catalytic properties of nanomaterials.Tuning surface strain is an effective strategy for enhancing catalytic activity;however,the correlation studies between the surface strain with catalytic performance are scant because such mechanistic studies require the precise control of surface strain on catalysts.In this work,a simple strategy of precisely tuning compressive surface strain of atomic-layer Cu2O on Cu@Ag (AL-Cu2O/Cu@Ag) nanoparticles (NPs) is demonstrated.The AL-Cu2O is synthesized by structure evolution of Cu@Ag core-shell nanoparticles,and the precise thickness-control of AL-Cu2O is achieved by tuning the molar ratio of Cu/Ag of the starting material.Aberration-corrected high-resolution transmission electron microscopy (AC-HRTEM) and EELS elemental mapping characterization showed that the compressive surface strain of AL-Cu2O along the [111] and [200] directions can be precisely tuned from 6.5% to 1.6% and 6.6% to 4.7%,respectively,by changing the number of AL-Cu2O layer from 3 to 6.The as-prepared AL-Cu2O/Cu@Ag NPs exhibited excellent catalytic property in the synthesis of azobenzene from aniline,in which the strained 4-layers Cu2O (4.5% along the [111] direction,6.1% along the [200] direction) exhibits the best catalytic performance.This work may be beneficial for the design and surface engineering of catalysts toward specific applications.
基金Supported by the National Natural Science Foundation of China under Grant Nos 10174081 and 60425411.
文摘Er2O3 thin films are grown on oxidized Si （111） substrates by molecular beam epitaxy. The sample grown under optimized condition is characterized in its microstructure, surface morphology and thickness using grazing incidence x-ray diffraction （GIXRD）, atomic force morphology and x-ray reflectivity. GIXRD measurements reveal that the Er2O3 thin film is a mosaic of single-crystal domains. The interplanar spacing d in-plane residual strain tensor ell and the strain relaxation degree ε are calculated. The Poisson ratio μ obtained by conventional x-ray diffraction is in good agreement with that of the bulk Er2O3. In-plane strains in three sets of planes, i.e. （440）, （404）, and （044）, are isotropic.
基金Project supported by the Zhejiang Provincial Natural Science Foundation,China(Grant Nos.LY16F040003 and LY16A040007)the National Natural Science Foundation of China(Grant Nos.51401069 and 11204058)
文摘In our experiment, an atomic layer MoS2structure grown on SiO2/Si substrates is used in transport test. The voltage U14,23 oscillates and the corresponding period varies with applied current. The largest period appears at 45 μA. The oscillation periods are different when samples are under laser radiation or in darkness. We discover that under the laser irradiation, the oscillation period occurs at lower current than in the darkness case. Meanwhile, the drift velocity is estimated at ~10~7 cm/s. Besides, by studying the envelope of U14,23 versus applied current, we see a beating phenomenon at a certain current value. The beating period in darkness is larger than under laser irradiation. The difference between beating periods reveals the energy difference of electrons. Similar results are obtained by using different laser power densities and different light sources. The possible mechanism behind the oscillation period is discussed.
基金supported by the National Key Research and Development Program of China(Grant Nos.2022YFA1402404 and 2023YFA1406304)the National Natural Science Foundation of China(Grant Nos.92161201,T2221003,12104221,12104220,12274208,12025404,12004174,91961101,62274085,12374043,and U2032208)+2 种基金the Natural Science Foundation of Jiangsu Province(Grant Nos.BK20230079,BK20243013,and BK20233001)the Fundamental and Interdisciplinary Disciplines Breakthrough Plan of the Ministry of Education of China(No.JYB2025XDXM411)the Fundamental Research Funds for the Central Universities(Grant Nos.020414380192 and 2024300432).
文摘The nonlinear Hall effect(NLHE)has attracted extensive attention due to its complex physical origins and rectification characteristics with time-reversal symmetry.However,the special symmetry requirements have restricted the research and application of NLHE.Here we have developed an in-situ on-device electrochemical intercalation method to fabricate cetyltrimethylammonium cation(CTA^(+))intercalated MoS_(2) device.Structural characterization demonstrates that owing to the intercalation of CTA+,the atomic structure within the layers remains unchanged,but the layer distance expands from 0.61 nm to 1.06 nm,distinguish with the previous research.Due to the substantial injection of electrons by the intercalation process,the transport behavior of MoS_(2) transforms from semi-metallic to metallic.By breaking of inversion symmetry introduced by the intercalation of CTA^(+),NLHE is induced.In the measurement of temperature-dependent NLHE,not only the main mechanism of skew scattering is confirmed by the nonlinear susceptibility analysis,but also a significant NLHE with the second-harmonic nonlinear Hall coefficient can be still observed under room temperature of 300 K.Our work expands the candidates of room-temperature NLHE materials and provides a new perspective for investigating the NLHE and symmetry engineering in two-dimensional materials.
