Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and t...Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD.展开更多
Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the devel...Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather challenging.Herein,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea production.Our results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic properties.Interestingly,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side reactions.The outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active sites.Our findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.展开更多
This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material tra...This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material transistor is simple and can be used to improve the quality of the interface of air-sensitive 2D materials.In comparison to HfS_(2) transistors utilizing a conventional Al_2O_(3) gate insulator by atomic layer deposition,HfS_(2) transistors utilizing an SAM as the gate dielectric can reduce the operation region from 4 V to 2 V,enhance the field-effect mobility from 0.03 cm^2/Vs to 0.75 cm^2/Vs,improve the sub-threshold swing from 404 m V/dec to 156 m V/dec,and optimize the hysteresis to 0.03 V,thus demonstrating improved quality of the semiconductor/insulator interface.展开更多
Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.Howev...Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.However, the photo-harvesting efficiency still requires improvement. In this study, A TMD stacked heterojunction structure was adopted to further enhance the performance of the PEC cathode. A P-type WSe_2 and an N-type Mo S_2 monolayer were stacked layer-by-layer to build a ultrathin vertical heterojunction using a micro-fabrication method.In situ measurement was employed to characterize the intrinsic PEC performance on a single-sheet heterostructure.Benefitting from its built-in electric field and type II band alignment, the MoS_2/WSe_2 bilayer heterojunction exhibited exceptional photocatalytic activity and a high incident photo-to-current conversion efficiency(IPCE). Comparing with the monolayer WSe_2 cathode, the PEC current and the IPCE of the bilayer heterojunction increased by a factor of 5.6 and enhanced 50%, respectively. The intriguing performance renders the MoS_2/WSe_2 heterojunction attractive for application in high-performance PEC water splitting.展开更多
Searching for two-dimensional（2 D） stable materials with direct band gap and high carrier mobility has attracted great attention for their electronic device applications.Using the first principles calculations and p...Searching for two-dimensional（2 D） stable materials with direct band gap and high carrier mobility has attracted great attention for their electronic device applications.Using the first principles calculations and particle swarm optimization（PSO） method,we predict a new 2 D stable material（HfNZ monolayer） with the global minimum of 2 D space.The HfNZ monolayer possesses direct band gap（～1.46 eV） and it is predicted to have high carrier mobilities(～103 cm2·V-1·s-1)from deformation potential theory.The direct band gap can be well maintained and flexibly modulated by applying an easily external strain under the strain conditions.In addition,the newly predicted HfN2 monolayer possesses good thermal,dynamical,and mechanical stabilities,which are verified by ab initio molecular dynamics simulations,phonon dispersion and elastic constants.These results demonstrate that HfN2 monolayer is a promising candidate in future microelectronic devices.展开更多
Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single a...Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.展开更多
To maximize the catalytic performance of MoS_(2) in the hydrogen evolution reaction,we investigate the electrocatalytic and photocatalytic performance of monolayer MoS_(2) doped with noble metal(Ag,Au,Cu,Pd,and Pt)usi...To maximize the catalytic performance of MoS_(2) in the hydrogen evolution reaction,we investigate the electrocatalytic and photocatalytic performance of monolayer MoS_(2) doped with noble metal(Ag,Au,Cu,Pd,and Pt)using first principles calculation combined with the climbing image nudged elastic band method.We find the band gap of the monolayer MoS_(2) is reduced significantly by the noble metal doping,which is unfavorable to improving its photocatalytic performance.The optical absorption coefficient shows that the doping does not increase the ability of the monolayer MoS_(2) to absorb visible light.The monolayer MoS_(2) doped with the noble metal is not a potential photocatalyst for the hydrogen evolution reaction because the band edge position of the conduction band minimum is lower than-4.44 eV,the reduction potential of H^(+)/H_(2).Fortunately,the band gap reduction increases the electron transport performance of the monolayer MoS_(2),and the activation energy of water splitting is greatly reduced by the noble metal doping,especially the Pt doping.On the whole,noble metal doping can enhance the electrocatalytic performance of the monolayer MoS_(2).展开更多
Entanglement is a defining feature of quantum physics with no classical analog. On the one hand, it is a powerful concept used in the fundamental study of quantum systems, many-body physics and even black hole physics...Entanglement is a defining feature of quantum physics with no classical analog. On the one hand, it is a powerful concept used in the fundamental study of quantum systems, many-body physics and even black hole physics. On the other hand, it is a key resource in quantum communication and information processing. Entanglement has been realized between photons[1], ions[2], spins[3], quantum dots[4] and even larger objects such as macroscopic diamonds[5]. Entanglement involving macroscopic objects is particularly intriguing and holds promise for novel quantum technologies. In a recent paper[6] published in Nature Physics, Srivastava and coworkers have unveiled an intriguing entanglement between collective and macroscopic vibration involving billions of atoms of the crystal (phonon) and a single optical excitation of a quantum dot (QD) in monolayer WSe2 (Fig. 1(a)). This is the first report on single photon entangled with phonon.展开更多
High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS...High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.展开更多
Dynamic processes of electron transfer by optical doping in monolayer MoSe2 at 6 K are investigated via measuring time resolved photoluminescence(PL)traces under different excitation powers.Time-dependent electron tra...Dynamic processes of electron transfer by optical doping in monolayer MoSe2 at 6 K are investigated via measuring time resolved photoluminescence(PL)traces under different excitation powers.Time-dependent electron transfer process can be analyzed by a power-law distribution of t^−α withα=0.1-0.24,depending on the laser excitation power.The average electron transfer time of approximately 27.65 s is obtained in the excitation power range of 0.5 to 100μW.As the temperature increases from 20 to 44 K,the energy difference between the neutral and charged excitons is observed to decrease.展开更多
Recently, two-dimensional monolayer molybdenum disulfide(MoS_2), a transition metal dichalcogenide, has received considerable attention due to its direct bandgap, which does not exist in its bulk form, enabling applic...Recently, two-dimensional monolayer molybdenum disulfide(MoS_2), a transition metal dichalcogenide, has received considerable attention due to its direct bandgap, which does not exist in its bulk form, enabling applications in optoelectronics and also thanks to its enhanced catalytic activity which allows it to be used for energy harvesting. However,growth of controllable and high-quality monolayers is still a matter of research and the parameters determining growth mechanism are not completely clear. In this work, chemical vapor deposition is utilized to grow monolayer MoS_2 flakes while deposition duration and temperature effect have been systematically varied to develop a better understanding of the MoS_2 film formation and the influence of these parameters on the quality of the monolayer flakes. Different from previous studies, SEM results show that single-layer MoS_2 flakes do not necessarily grow flat on the surface, but rather they can stay erect and inclined at different angles on the surface, indicating possible gas-phase reactions allowing for monolayer film formation. We have also revealed that process duration influences the amount of MoO_3/MoO_2 within the film network. The homogeneity and the number of layers depend on the change in the desorption–adsorption of radicals together with sulfurization rates, and, inasmuch, a careful optimization of parameters is crucial. Therefore, distinct from the general trend of MoS_2 monolayer formation, our films are rough and heterogeneous with monolayer MoS_2 nanowalls. Despite this roughness and the heterogeneity, we observe a strong photoluminescence located around 675 nm.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDs)have attracted considerable attention because of their unique properties and great potential in nano-technology applications.Great efforts have been devoted to ...Two-dimensional(2D)transition metal dichalcogenides(TMDs)have attracted considerable attention because of their unique properties and great potential in nano-technology applications.Great efforts have been devoted to fabrication of novel structured TMD monolayers by modifying their pristine structures at the atomic level.Here we propose an intriguing structured 1T-PtTe2 monolayer as hydrogen evolution reaction(HER)catalyst,namely,Pt4Te7,using first-principles calculations.It is found that Pt4Te7 is a stable monolayer material verified by the calculation of formation energy,phonon dispersion,and ab initio molecular dynamics simulations.Remarkably,the novel structured void-containing monolayer exhibits superior catalytic activity toward HER compared with the pristine one,with a Gibbs free energy very close to zero(less than 0.07 eV).These features indicate that Pt4Te7 monolayer is a high-performance HER catalyst with a high platinum utilization.These findings open new perspectives for the functionalization of 2D TMD materials at an atomic level and its application in HER catalysis.展开更多
To understand the dispersion behavior of metal oxides on composite oxide supports and with the expectation of developing more feasible catalysts for soot oxidation,CuO/La_(2)Sn_(2)O_(7)samples containing varied CuO lo...To understand the dispersion behavior of metal oxides on composite oxide supports and with the expectation of developing more feasible catalysts for soot oxidation,CuO/La_(2)Sn_(2)O_(7)samples containing varied CuO loadings were fabricated and characterized by different techniques and density functional theory calculations.In these catalysts,a spontaneous dispersion of CuO on the La_(2)Sn_(2)O_(7)pyrochlore support formed,having a monolayer dispersion capacity of 1.90 mmol CuO/100 m^(2) La_(2)Sn_(2)O_(7)surface.When loaded below this capacity,CuO exists in a sub-monolayer or monolayer state.X-ray photoelectron spectroscopy(XPS),Raman spectroscopy,and Bader charge and density of states analyses indicate that there are strong interactions between the sub-monolayer/monolayer CuO and the La_(2)Sn_(2)O_(7)support,mainly through the donation of electrons from Cu to Sn at the B-sites of the structure.In contrast,Cu has negligible interactions with La at the A-sites.This suggests that,in composite oxide supports containing multiple metals,the supported metal oxide interacts preferentially with one kind of metal cation in the support.The Raman,in situ diffuse reflectance infrared Fourier transform spectroscopy,and XPS results confirmed the formation of both O2^(-)and O2^(2-)as the active sites on the surfaces of the CuO/La_(2)Sn_(2)O_(7)catalysts,and the concentration of these active species determines the soot combustion activity.The number of active oxygen anions increased with increase in CuO loading until the monolayer dispersion capacity was reached.Above the monolayer dispersion capacity,microsized CuO crystallites formed,and these had a negative effect on the generation of active surface oxygen sites.In summary,a highly active catalyst can be prepared by covering the surface of the La_(2)Sn_(2)O_(7)support with a CuO monolayer.展开更多
Monolayer MoS_(2)has a promising optoelectronics property,with a bandgap in the visible range;the material is a potential candidate for solar cell applications.In this work,we grew MoS_(2)monolayers using a low-pressu...Monolayer MoS_(2)has a promising optoelectronics property,with a bandgap in the visible range;the material is a potential candidate for solar cell applications.In this work,we grew MoS_(2)monolayers using a low-pressure chemical vapor deposition approach.To produce uniform wafer-scale MoS_(2)monolayer films,precursors molybdenum dioxide(MoO_(2))and sulfur(S)are utilized.Atomic force microscopy was used to quantify the thickness of the monolayers,and the result was validated by Raman spectroscopy.Transmission electron microscopy(TEM)was used to confirm the crystalline quality of the monolayers,and photoluminescence spectroscopy was used to evaluate their optical properties.We were able to create a Schottky solar cell with a MoS_(2)monolayer up to 1 cm2 area by transferring monolayer film to n-type silicon.The MoS_(2)/n-Si Schottky solar cell demonstrated photovoltaic characteristics with a short circuit current density of 14.8 mA cm^(-2)and an open-circuit voltage of 0.32 V under 100 mW cm^(-2)illumination.The fill factor and energy conversion efficiency were 53%and 2.46%,respectively,with the highest external quantum efficiency at 530 nm being 44%.展开更多
基金supported by National Research Foundation of Korea (NRF)funded by the Ministry of Education (2021R1A6A1A03039696,2022R1A2C2009412)
文摘Two-dimensional(2D)transition metal dichalcogenides(TMD)are atomically thin semiconductors with promising optoelectronic applications across the visible spectrum.However,their intrinsically weak light absorption and the low photoluminescence quantum yield(PLQY)restrict their performance and potential use,especially in ultraviolet(UV)wavelength light ranges.Quantum dots(QD)derived from 2D materials(2D/QD)provide efficient light absorption and emission of which energy can be tuned for desirable light wavelength.In this study,we greatly enhanced the photon absorption and PLQY of monolayer(1L)tungsten disulfide(WS_(2))in the UV range via hybridization with 2D/QD,particularly titanium nitride MXene QD(Ti_(2)N MQD)and graphitic carbon nitride QD(GCNQD).With the hybridization of MQD or GCNQD,1LWS_(2)showed a maximum PL enhancement by 15 times with 300 nm wavelength excitation,while no noticeable enhancement was observed when the excitation photon energy was less than the bandgap of the QD,indicating that UV absorption by the QD played a crucial role in enhancing the light emission of 1L-WS_(2)in our 0D/2D hybrid system.Our findings present a convenient method for enhancing the photo-response of 1L-WS_(2)to UV light and offer exciting possibilities for harvesting UV energy using 1L-TMD.
基金financially supported in China by Natural Science Funds for Distinguished Young Scholars of Heilongjiang Province(No.JC2018004)Natural Science Foundation of Heilongjiang Province of China(No.TD2020B001)in the USA by NSF-CREST Center for Innovation,Research,and Education in Environmental Nanotechnology(CIRE2N)(No.HRD-1736093)
文摘Urea synthesis through the simultaneous electrocatalytic reduction of N_(2)and CO_(2)molecules under ambient conditions holds great promises as a sustainable alternative to its industrial production,in which the development of stable,highly efficient,and highly selective catalysts to boost the chemisorption,activation,and coupling of inert N_(2)and CO_(2)molecules remains rather challenging.Herein,by means of density functional theory computations,we proposed a new class of two-dimensional nanomaterials,namely,transition-metal phosphide monolayers(TM_(2)P,TM=Ti,Fe,Zr,Mo,and W),as the potential electrocatalysts for urea production.Our results showed that these TM_(2)P materials exhibit outstanding stability and excellent metallic properties.Interestingly,the Mo_(2)P monolayer was screened out as the best catalyst for urea synthesis due to its small kinetic energy barrier(0.35 eV)for C-N coupling,low limiting potential(-0.39 V),and significant suppressing effects on the competing side reactions.The outstanding catalytic activity of the Mo_(2)P monolayer can be ascribed to its optimal adsorption strength with the key^(*)NCON species due to its moderate positive charges on the Mo active sites.Our findings not only propose a novel catalyst with high-efficiency and high-selectivity for urea production but also further widen the potential applications of metal phosphides in electrocatalysis.
基金Supported by the Japan Society for the Promotion of Science under Grant No JP25107004
文摘This work details a study based on HfS_(2 )transistors utilizing an n-octadecylphosphonic acid-based self-assembled monolayer(SAM)as the gate dielectric.The fabrication of the SAM-based two-dimensional(2D)material transistor is simple and can be used to improve the quality of the interface of air-sensitive 2D materials.In comparison to HfS_(2) transistors utilizing a conventional Al_2O_(3) gate insulator by atomic layer deposition,HfS_(2) transistors utilizing an SAM as the gate dielectric can reduce the operation region from 4 V to 2 V,enhance the field-effect mobility from 0.03 cm^2/Vs to 0.75 cm^2/Vs,improve the sub-threshold swing from 404 m V/dec to 156 m V/dec,and optimize the hysteresis to 0.03 V,thus demonstrating improved quality of the semiconductor/insulator interface.
基金supported by the National Natural Science Foundation of China (Grant Nos.51290271,51672314)the Guangdong Natural Science Foundation (Grant No.2016A030313359)+2 种基金the Science and Technology Program of Guangzhou (Grant No.201707010224)the Science and Technology Department of Guangdong Provincethe Fundamental Research Funds for the Central Universities
文摘Transition-metal dichalcogenide(TMD) semiconductors have attracted interest as photoelectrochemical(PEC) electrodes due to their novel band-gap structures,optoelectronic properties, and photocatalytic activities.However, the photo-harvesting efficiency still requires improvement. In this study, A TMD stacked heterojunction structure was adopted to further enhance the performance of the PEC cathode. A P-type WSe_2 and an N-type Mo S_2 monolayer were stacked layer-by-layer to build a ultrathin vertical heterojunction using a micro-fabrication method.In situ measurement was employed to characterize the intrinsic PEC performance on a single-sheet heterostructure.Benefitting from its built-in electric field and type II band alignment, the MoS_2/WSe_2 bilayer heterojunction exhibited exceptional photocatalytic activity and a high incident photo-to-current conversion efficiency(IPCE). Comparing with the monolayer WSe_2 cathode, the PEC current and the IPCE of the bilayer heterojunction increased by a factor of 5.6 and enhanced 50%, respectively. The intriguing performance renders the MoS_2/WSe_2 heterojunction attractive for application in high-performance PEC water splitting.
基金Project supported by the National Natural Science Foundation(Grant No.U1404108)the Innovative Talents of Universities in Henan Province of China(Grant No.17HASTIT013)+1 种基金the Basic and Frontier Technology Research Program of Henan Province of China(Grant No.162300410056)the Key Scientific Research Projects of Higher Institutions in Henan Province of China(Grant No.19A140018).
文摘Searching for two-dimensional（2 D） stable materials with direct band gap and high carrier mobility has attracted great attention for their electronic device applications.Using the first principles calculations and particle swarm optimization（PSO） method,we predict a new 2 D stable material（HfNZ monolayer） with the global minimum of 2 D space.The HfNZ monolayer possesses direct band gap（～1.46 eV） and it is predicted to have high carrier mobilities(～103 cm2·V-1·s-1)from deformation potential theory.The direct band gap can be well maintained and flexibly modulated by applying an easily external strain under the strain conditions.In addition,the newly predicted HfN2 monolayer possesses good thermal,dynamical,and mechanical stabilities,which are verified by ab initio molecular dynamics simulations,phonon dispersion and elastic constants.These results demonstrate that HfN2 monolayer is a promising candidate in future microelectronic devices.
文摘Formaldehyde(HCHO) is a common indoor pollutant, long-term exposure to HCHO may harm human health. Its efficient removal at mild conditions is still challenging. The catalytic oxidation of HCHO molecules on a single atomic catalyst, Ti-decorated Ti3C2O2(Ti/Ti3C2O2) monolayer, is investigated by performing the first principles calculations in this work. It demonstrates that Ti atoms can be easily well dispersed at the form of single atom on Ti3C2O2 monolayer without aggregation. For HCHO catalytic oxidation, both Langmuir-Hinshelwood(LH) and Eley-Rideal(ER) mechanisms are considered. The results show that the step of HCHO dissociative adsorption on Ti/Ti3C2O2 with activated O2 can release high energy of 4.05 e V based on the ER mechanism, which can help to overcome the energy barrier(1.04 e V) of the subsequent reaction steps. The charge transfer from *OH group to CO molecule(dissociated from HCHO) not only promotes *OH group activation but also plays an important role in the H2 O generation along the ER mechanism. Therefore, HCHO can be oxidized easily on Ti/Ti3C2O2 monolayer, this work could provide significant guidance to develop effective non-noble metal catalysts for HCHO oxidation and broaden the applications of MXene-based materials.
基金the Joint Funds of the National Natural Science Foundation of China(Grant No.U1967212)the National Science and Technology Major Project of China(Grant No.2019XS06004009)the Fundamental Research Funds for the Central Universities(Grant No.2018ZD10).
文摘To maximize the catalytic performance of MoS_(2) in the hydrogen evolution reaction,we investigate the electrocatalytic and photocatalytic performance of monolayer MoS_(2) doped with noble metal(Ag,Au,Cu,Pd,and Pt)using first principles calculation combined with the climbing image nudged elastic band method.We find the band gap of the monolayer MoS_(2) is reduced significantly by the noble metal doping,which is unfavorable to improving its photocatalytic performance.The optical absorption coefficient shows that the doping does not increase the ability of the monolayer MoS_(2) to absorb visible light.The monolayer MoS_(2) doped with the noble metal is not a potential photocatalyst for the hydrogen evolution reaction because the band edge position of the conduction band minimum is lower than-4.44 eV,the reduction potential of H^(+)/H_(2).Fortunately,the band gap reduction increases the electron transport performance of the monolayer MoS_(2),and the activation energy of water splitting is greatly reduced by the noble metal doping,especially the Pt doping.On the whole,noble metal doping can enhance the electrocatalytic performance of the monolayer MoS_(2).
文摘Entanglement is a defining feature of quantum physics with no classical analog. On the one hand, it is a powerful concept used in the fundamental study of quantum systems, many-body physics and even black hole physics. On the other hand, it is a key resource in quantum communication and information processing. Entanglement has been realized between photons[1], ions[2], spins[3], quantum dots[4] and even larger objects such as macroscopic diamonds[5]. Entanglement involving macroscopic objects is particularly intriguing and holds promise for novel quantum technologies. In a recent paper[6] published in Nature Physics, Srivastava and coworkers have unveiled an intriguing entanglement between collective and macroscopic vibration involving billions of atoms of the crystal (phonon) and a single optical excitation of a quantum dot (QD) in monolayer WSe2 (Fig. 1(a)). This is the first report on single photon entangled with phonon.
基金financially supported by Shenzhen Key Laboratory of Advanced Energy Storage(No.ZDSYS20220401141000001)the Research Grants Council of the Hong Kong Special Administrative Region,China(Project No.R6005-20)。
文摘High theoretical capacity and unique layered structures make MoS_(2)a promising lithium-ion battery anode material.However,the anisotropic ion transport in layered structures and the poor intrinsic conductivity of MoS_(2)lead to unacceptable ion transport capability.Here,we propose in-situ construction of interlayer electrostatic repulsion caused by Co^(2+)substituting Mo^(4+)between MoS_(2)layers,which can break the limitation of interlayer van der Waals forces to fabricate monolayer MoS_(2),thus establishing isotropic ion transport paths.Simultaneously,the doped Co atoms change the electronic structure of monolayer MoS_(2),thus improving its intrinsic conductivity.Importantly,the doped Co atoms can be converted into Co nanoparticles to create a space charge region to accelerate ion transport.Hence,the Co-doped monolayer MoS_(2)shows ultrafast lithium ion transport capability in half/full cells.This work presents a novel route for the preparation of monolayer MoS_(2)and demonstrates its potential for application in fast-charging lithium-ion batteries.
基金supported by the National Natural Science Foundation of China under Grant Nos 61674135,11974342 and 61827823.
文摘Dynamic processes of electron transfer by optical doping in monolayer MoSe2 at 6 K are investigated via measuring time resolved photoluminescence(PL)traces under different excitation powers.Time-dependent electron transfer process can be analyzed by a power-law distribution of t^−α withα=0.1-0.24,depending on the laser excitation power.The average electron transfer time of approximately 27.65 s is obtained in the excitation power range of 0.5 to 100μW.As the temperature increases from 20 to 44 K,the energy difference between the neutral and charged excitons is observed to decrease.
基金supported by Anadolu University BAP 1407F335 and BAP 1505F271 Projects
文摘Recently, two-dimensional monolayer molybdenum disulfide(MoS_2), a transition metal dichalcogenide, has received considerable attention due to its direct bandgap, which does not exist in its bulk form, enabling applications in optoelectronics and also thanks to its enhanced catalytic activity which allows it to be used for energy harvesting. However,growth of controllable and high-quality monolayers is still a matter of research and the parameters determining growth mechanism are not completely clear. In this work, chemical vapor deposition is utilized to grow monolayer MoS_2 flakes while deposition duration and temperature effect have been systematically varied to develop a better understanding of the MoS_2 film formation and the influence of these parameters on the quality of the monolayer flakes. Different from previous studies, SEM results show that single-layer MoS_2 flakes do not necessarily grow flat on the surface, but rather they can stay erect and inclined at different angles on the surface, indicating possible gas-phase reactions allowing for monolayer film formation. We have also revealed that process duration influences the amount of MoO_3/MoO_2 within the film network. The homogeneity and the number of layers depend on the change in the desorption–adsorption of radicals together with sulfurization rates, and, inasmuch, a careful optimization of parameters is crucial. Therefore, distinct from the general trend of MoS_2 monolayer formation, our films are rough and heterogeneous with monolayer MoS_2 nanowalls. Despite this roughness and the heterogeneity, we observe a strong photoluminescence located around 675 nm.
基金Project supported by the National Key R&D Program of China(Grant Nos.2016YFA0202300,2018YFA0305800,and 2019YFA0308500)the National Natural Science Foundation of China(Grant Nos.61888102,51872284,and 51922011)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB30000000).
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDs)have attracted considerable attention because of their unique properties and great potential in nano-technology applications.Great efforts have been devoted to fabrication of novel structured TMD monolayers by modifying their pristine structures at the atomic level.Here we propose an intriguing structured 1T-PtTe2 monolayer as hydrogen evolution reaction(HER)catalyst,namely,Pt4Te7,using first-principles calculations.It is found that Pt4Te7 is a stable monolayer material verified by the calculation of formation energy,phonon dispersion,and ab initio molecular dynamics simulations.Remarkably,the novel structured void-containing monolayer exhibits superior catalytic activity toward HER compared with the pristine one,with a Gibbs free energy very close to zero(less than 0.07 eV).These features indicate that Pt4Te7 monolayer is a high-performance HER catalyst with a high platinum utilization.These findings open new perspectives for the functionalization of 2D TMD materials at an atomic level and its application in HER catalysis.
文摘To understand the dispersion behavior of metal oxides on composite oxide supports and with the expectation of developing more feasible catalysts for soot oxidation,CuO/La_(2)Sn_(2)O_(7)samples containing varied CuO loadings were fabricated and characterized by different techniques and density functional theory calculations.In these catalysts,a spontaneous dispersion of CuO on the La_(2)Sn_(2)O_(7)pyrochlore support formed,having a monolayer dispersion capacity of 1.90 mmol CuO/100 m^(2) La_(2)Sn_(2)O_(7)surface.When loaded below this capacity,CuO exists in a sub-monolayer or monolayer state.X-ray photoelectron spectroscopy(XPS),Raman spectroscopy,and Bader charge and density of states analyses indicate that there are strong interactions between the sub-monolayer/monolayer CuO and the La_(2)Sn_(2)O_(7)support,mainly through the donation of electrons from Cu to Sn at the B-sites of the structure.In contrast,Cu has negligible interactions with La at the A-sites.This suggests that,in composite oxide supports containing multiple metals,the supported metal oxide interacts preferentially with one kind of metal cation in the support.The Raman,in situ diffuse reflectance infrared Fourier transform spectroscopy,and XPS results confirmed the formation of both O2^(-)and O2^(2-)as the active sites on the surfaces of the CuO/La_(2)Sn_(2)O_(7)catalysts,and the concentration of these active species determines the soot combustion activity.The number of active oxygen anions increased with increase in CuO loading until the monolayer dispersion capacity was reached.Above the monolayer dispersion capacity,microsized CuO crystallites formed,and these had a negative effect on the generation of active surface oxygen sites.In summary,a highly active catalyst can be prepared by covering the surface of the La_(2)Sn_(2)O_(7)support with a CuO monolayer.
文摘Monolayer MoS_(2)has a promising optoelectronics property,with a bandgap in the visible range;the material is a potential candidate for solar cell applications.In this work,we grew MoS_(2)monolayers using a low-pressure chemical vapor deposition approach.To produce uniform wafer-scale MoS_(2)monolayer films,precursors molybdenum dioxide(MoO_(2))and sulfur(S)are utilized.Atomic force microscopy was used to quantify the thickness of the monolayers,and the result was validated by Raman spectroscopy.Transmission electron microscopy(TEM)was used to confirm the crystalline quality of the monolayers,and photoluminescence spectroscopy was used to evaluate their optical properties.We were able to create a Schottky solar cell with a MoS_(2)monolayer up to 1 cm2 area by transferring monolayer film to n-type silicon.The MoS_(2)/n-Si Schottky solar cell demonstrated photovoltaic characteristics with a short circuit current density of 14.8 mA cm^(-2)and an open-circuit voltage of 0.32 V under 100 mW cm^(-2)illumination.The fill factor and energy conversion efficiency were 53%and 2.46%,respectively,with the highest external quantum efficiency at 530 nm being 44%.
