It is found that several layer-phase group-III monochalcogenides, including GaS, GaSe, and InSe, are piezoelectric in their monolayer form. First-principles calculations reveal that the piezoelectric coefficients of m...It is found that several layer-phase group-III monochalcogenides, including GaS, GaSe, and InSe, are piezoelectric in their monolayer form. First-principles calculations reveal that the piezoelectric coefficients of monolayer GaS, GaSe, and InSe （2.06, 2.30, and 1.46 pm-V-1） are of the same order of magnitude as previously discovered two-dimensional （2D） piezoelectric materials such as boron nitride （BN） and MoS2 monolayers. This study therefore indicates that a strong piezoelectric response can be obtained in a wide range of two-dimensional materials with broken inversion symmetry. The co-existence of piezoelectricity and superior photo-sensitivity in these monochalcogenide monolayer semiconductors means they have the potential to allow for the integration of electromechanical and optical sensors on the same material platform.展开更多
Investigating the promising chalcogenide materials for the development of memory and advanced neuromorphic computing applications is a critical step in realizing electronic memory and synaptic devices that can efficie...Investigating the promising chalcogenide materials for the development of memory and advanced neuromorphic computing applications is a critical step in realizing electronic memory and synaptic devices that can efficiently emulate biological synaptic functions.However,the assessment of monochalcogenide materials for the fabrication of highly scalable memory and electronic synaptic devices that can accurately mimic synaptic functions remain limited.In the present study,we investigated the thickness-dependent resistive switching(RS)behavior of conductive bridge random access memory(CBRAM)based on a monochalcogenide GeSe switching medium for its possible application in high-performance memory and electronic synapses.GeSe thin films of different thicknesses(6,13,24,35,47,and 56 nm)were deposited via sputtering to fabricate CBRAM devices with a stacking sequence of Ag/GeSe/Pt/Ti/SiO_(2).The devices exhibited compliance current(CC)-free and electroforming-free RS with highly stable endurance and retention characteristics with no major degradation.All devices with a thickness of 6 nm had a low-resistance state(LRS),which required an initial reset to ensure reliable switching cycles.The devices with a thickness of 47 nm and above exhibited the co-existence of unipolar resistive switching(U-RS)and bipolar resistive switching(B-RS)with the CC-controlled transition between the two switching behaviors.Multilevel resistance states in the 24-nm device between a high-resistance state(HRS)and an LRS were achieved by controlling the set-CC(from 5 mA to CC-free)and the reset stop voltage(from–0.5 to–1.0 V)during the set and reset processes,respectively.The analog RS behavior of the device was further investigated with appropriate pulse measurements to emulate vital synaptic functions,including long-term potentiation(LTP),long-term depression(LTD),spike-rate-dependent plasticity(SRDP),spike-timing-dependent plasticity(STDP),paired-pulse facilitation(PPF),paired-pulse depression(PPD)and post-tetanic potentiation(PTP).Overall,the detailed investigation of thickness-dependent GeSe monochalcogenide material indicates that it is a highly suitable candidate for use in highly scalable memory devices and electronic synapses for neuromorphic computing applications.展开更多
On the basis of known structures of 13-GeTe bulk and the derived monolayer,we proposed a series of structural analogues MXs(M=Ge,Sn;X=S,Se,Te)with an intrinsic built-in electric field via a substitution strategy.Using...On the basis of known structures of 13-GeTe bulk and the derived monolayer,we proposed a series of structural analogues MXs(M=Ge,Sn;X=S,Se,Te)with an intrinsic built-in electric field via a substitution strategy.Using first-principles calculations,we demonstrated that these MX monolayers and bulks are thermodynamically,dynamically and mechanically stable,and the stabilities of bulks are more robust than the monolayer counterparts.Electronic calculations showed that the monolayers have large band gaps ranging from 2.38 to 3.27 eV while the bulks have pronounced small band gaps ranging from 0.06 to 0.78 eV.The calculated piezoelectric coefficients d11 for the MX monolayers are in the range from 6.6 to 10.9 pmN.Strikingly,the calculated d33 for the MX bulks are as high as 40.3-213.7 pm/V.By correlating atomic polarizability,atomic mass,relative ion motion,Bader charge and lattice parameters,we proposed an empirical model to estimate the piezoelectric coefficients for the two-dimensional:(2D)MXs,where a nice match between the estimated ones and the calculated ones was found.The versatile electronic propertiesand large piezoelectric coefficients endow MXs a broad prospect of application in optoelectronic and piezoelectric devices,and the revealed underlying mechanisms offer valuable guidelines for seeking novel piezoelectrics.展开更多
Piezoelectricity is pivotal for applications in micro/nanoelectromechanical systems(MEMS/NEMS).Inducing such a property in 2D systems via the reduction of the dimensionality of their corresponding 3D bulk is here expl...Piezoelectricity is pivotal for applications in micro/nanoelectromechanical systems(MEMS/NEMS).Inducing such a property in 2D systems via the reduction of the dimensionality of their corresponding 3D bulk is here explored.Based on DFT theory and Gaussian-type-localized basis sets,the structural,electronic,mechanical,and piezoelectric properties of both 3D and 2D rare earth monochalcogenides RmX(Rm=Tm,Yb,Lu,and X=S,Se,Te)are investigated using the CRYSTAL code.Most intriguingly,the 2D LuX compounds display a buckled structure,where the Lu and X atoms protrude from the monolayer surface leading to an additional out-of-plane piezoelectric effect;(e_(31)=2104.84,1770.28,1689.79 pC/m,and d31=56.37,49.76,and 147.90 pm/V for LuS,LuSe,and LuTe,respectively).Such piezoelectric response is two orders of magnitude larger than the one of recently reported 2D ferroelectric MXenes,and is nearly thirty times larger than the commonly used AlN and GaN bulk structures.Furthermore,the reduced elastic constants obtained,when compared to other 2D materials,confirm the flexibility and softness of the considered 2D systems.展开更多
Photocatalytic water splitting utilizing solar energy is considered as one of the most ideal strategies for solving the ene rgy and environmental issues.Recently,two-dimensional(2 D)materials with an intrinsic dipole ...Photocatalytic water splitting utilizing solar energy is considered as one of the most ideal strategies for solving the ene rgy and environmental issues.Recently,two-dimensional(2 D)materials with an intrinsic dipole show great chance to achieve excellent photocatalytic performance.In this work,blue-phase monolayer carbon monochalcogenides(CX,X=S,Se)are constructed and systematically studied as photocatalysts for water splitting by performing first-principles calculations based on density functional theory.After confirming the great dynamical,thermal,and mechanical stability of CX monolayers,we observe that they possess moderate band gaps(2.41 eV for CS and 2.46 eV for CSe)and high carrier mobility(3.23×10^(4)cm^(2)V^(^(-1))s^(-1)for CS and 4.27×10^(3)cm^(2)V^(-1)s^(-1)for CSe),comparable to those of many recently reported 2 D photocatalysts.Moreover,these two monolayer materials are found to have large intrinsic dipole(0.43 D for CS and 0.51 D for CSe),thus the build-in internal electric field can be selfintroduced,which can effectively drive the separation of photongenerated carriers.More importantly,the well-aligned band edge as well as rather pronounced optical absorption in the visible-light and ultraviolet regions further ensure that our proposed CX monolayers can be used as high efficient photocatalysts for water splitting.Additionally,the effects of external strain on the electronic,optical and photocatalytic properties of CX monolayers are also evaluated.These theoretical predictions will stimulate further work to open up the energy-related applications of CX monolayers.展开更多
Two-dimensional honeycomb lattices show great potential in the realization of Dirac nodal line fermions(DNLFs).Here,we successfully synthesized a gold telluride(AuTe)monolayer by direct tellurizing an Au(111)substrate...Two-dimensional honeycomb lattices show great potential in the realization of Dirac nodal line fermions(DNLFs).Here,we successfully synthesized a gold telluride(AuTe)monolayer by direct tellurizing an Au(111)substrate.Low energy electron diffraction measurements reveal that it is(2×2)AuTe layer stacked onto(3×3)Au(111)substrate.Moreover,scanning tunneling microscopy images show that the AuTe layer has a honeycomb structure.Scanning transmission electron microscopy reveals that it is a single-atom layer.In addition,first-principles calculations demonstrate that the honeycomb AuTe monolayer exhibits Dirac nodal line features protected by mirror symmetry,which is validated by angle-resolved photoemission spectra.Our results establish that monolayer AuTe can be a good candidate to investigate 2D DNLFs and provides opportunities to realize high-speed low-dissipation devices.展开更多
GroupqV monochalcogenides are emerging as a new class of layered materials beyond graphene, transition metal dichalcogenides （TMDCs）, and black phosphorus （BP）. In this paper, we report experimental and theoretica...GroupqV monochalcogenides are emerging as a new class of layered materials beyond graphene, transition metal dichalcogenides （TMDCs）, and black phosphorus （BP）. In this paper, we report experimental and theoretical investigations of the band structure and transport properties of GeSe and its heterostructures. We find that GeSe exhibits a markedly anisotropic electronic transport, with maximum conductance along the armchair direction. Density functional theory calculations reveal that the effective mass is 2.7 times larger along the zigzag direction than the armchair direction; this mass anisotropy explains the observed anisotropic conductance. The crystallographic orientation of GeSe is confirmed by angle- resolved polarized Raman measurements, which are further supported by calculated Raman tensors for the orthorhombic structure. Novel GeSeflVIoS2 p-n heterojunctions are fabricated, combining the natural p-type doping in GeSe and n-type doping in MoS2. The temperature dependence of the measured junction current reveals that GeSe and MoS2 have a type-II band alignment with a conduction band offset of N 0.234 eV. The anisotropic conductance of GeSe may enable the development of new electronic and optoelectronic devices, such as high-efficiency thermoelectric devices and plasmonic devices with resonance frequency continuously tunable through light polarization direction. The unique GeSe/MoS2 p-n junctions with type-II alignment may become essential building blocks of vertical tunneling field-effect transistors for low-power applications. The novel p-type layered material GeSe can also be combined with n-type TMDCs to form heterogeneous complementary metal oxide semiconductor （CMOS） circuits.展开更多
文摘It is found that several layer-phase group-III monochalcogenides, including GaS, GaSe, and InSe, are piezoelectric in their monolayer form. First-principles calculations reveal that the piezoelectric coefficients of monolayer GaS, GaSe, and InSe （2.06, 2.30, and 1.46 pm-V-1） are of the same order of magnitude as previously discovered two-dimensional （2D） piezoelectric materials such as boron nitride （BN） and MoS2 monolayers. This study therefore indicates that a strong piezoelectric response can be obtained in a wide range of two-dimensional materials with broken inversion symmetry. The co-existence of piezoelectricity and superior photo-sensitivity in these monochalcogenide monolayer semiconductors means they have the potential to allow for the integration of electromechanical and optical sensors on the same material platform.
基金the Nano Material Technology Development Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT&Future Planning(Nos.2016M3A7B4909942 and 2016R1D1A1B01015047 as well by National Research Foundation of Korea(NRF)No.2020R1A6A1A03043435)the Nano Material Technology Development Programs and Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Science,ICT&Future Planning(Nos.NRF-2019R1F1A1057243 and NRF-2020M3F3A2A02082449).
文摘Investigating the promising chalcogenide materials for the development of memory and advanced neuromorphic computing applications is a critical step in realizing electronic memory and synaptic devices that can efficiently emulate biological synaptic functions.However,the assessment of monochalcogenide materials for the fabrication of highly scalable memory and electronic synaptic devices that can accurately mimic synaptic functions remain limited.In the present study,we investigated the thickness-dependent resistive switching(RS)behavior of conductive bridge random access memory(CBRAM)based on a monochalcogenide GeSe switching medium for its possible application in high-performance memory and electronic synapses.GeSe thin films of different thicknesses(6,13,24,35,47,and 56 nm)were deposited via sputtering to fabricate CBRAM devices with a stacking sequence of Ag/GeSe/Pt/Ti/SiO_(2).The devices exhibited compliance current(CC)-free and electroforming-free RS with highly stable endurance and retention characteristics with no major degradation.All devices with a thickness of 6 nm had a low-resistance state(LRS),which required an initial reset to ensure reliable switching cycles.The devices with a thickness of 47 nm and above exhibited the co-existence of unipolar resistive switching(U-RS)and bipolar resistive switching(B-RS)with the CC-controlled transition between the two switching behaviors.Multilevel resistance states in the 24-nm device between a high-resistance state(HRS)and an LRS were achieved by controlling the set-CC(from 5 mA to CC-free)and the reset stop voltage(from–0.5 to–1.0 V)during the set and reset processes,respectively.The analog RS behavior of the device was further investigated with appropriate pulse measurements to emulate vital synaptic functions,including long-term potentiation(LTP),long-term depression(LTD),spike-rate-dependent plasticity(SRDP),spike-timing-dependent plasticity(STDP),paired-pulse facilitation(PPF),paired-pulse depression(PPD)and post-tetanic potentiation(PTP).Overall,the detailed investigation of thickness-dependent GeSe monochalcogenide material indicates that it is a highly suitable candidate for use in highly scalable memory devices and electronic synapses for neuromorphic computing applications.
基金supported by the National Natural Science Foundation of China(No.1573002)Natural Science Funds for Distinguished Young Scholar of Anhui Province(No.1908085J08)。
文摘On the basis of known structures of 13-GeTe bulk and the derived monolayer,we proposed a series of structural analogues MXs(M=Ge,Sn;X=S,Se,Te)with an intrinsic built-in electric field via a substitution strategy.Using first-principles calculations,we demonstrated that these MX monolayers and bulks are thermodynamically,dynamically and mechanically stable,and the stabilities of bulks are more robust than the monolayer counterparts.Electronic calculations showed that the monolayers have large band gaps ranging from 2.38 to 3.27 eV while the bulks have pronounced small band gaps ranging from 0.06 to 0.78 eV.The calculated piezoelectric coefficients d11 for the MX monolayers are in the range from 6.6 to 10.9 pmN.Strikingly,the calculated d33 for the MX bulks are as high as 40.3-213.7 pm/V.By correlating atomic polarizability,atomic mass,relative ion motion,Bader charge and lattice parameters,we proposed an empirical model to estimate the piezoelectric coefficients for the two-dimensional:(2D)MXs,where a nice match between the estimated ones and the calculated ones was found.The versatile electronic propertiesand large piezoelectric coefficients endow MXs a broad prospect of application in optoelectronic and piezoelectric devices,and the revealed underlying mechanisms offer valuable guidelines for seeking novel piezoelectrics.
文摘Piezoelectricity is pivotal for applications in micro/nanoelectromechanical systems(MEMS/NEMS).Inducing such a property in 2D systems via the reduction of the dimensionality of their corresponding 3D bulk is here explored.Based on DFT theory and Gaussian-type-localized basis sets,the structural,electronic,mechanical,and piezoelectric properties of both 3D and 2D rare earth monochalcogenides RmX(Rm=Tm,Yb,Lu,and X=S,Se,Te)are investigated using the CRYSTAL code.Most intriguingly,the 2D LuX compounds display a buckled structure,where the Lu and X atoms protrude from the monolayer surface leading to an additional out-of-plane piezoelectric effect;(e_(31)=2104.84,1770.28,1689.79 pC/m,and d31=56.37,49.76,and 147.90 pm/V for LuS,LuSe,and LuTe,respectively).Such piezoelectric response is two orders of magnitude larger than the one of recently reported 2D ferroelectric MXenes,and is nearly thirty times larger than the commonly used AlN and GaN bulk structures.Furthermore,the reduced elastic constants obtained,when compared to other 2D materials,confirm the flexibility and softness of the considered 2D systems.
基金supported by the National Natural Science Foundation of China(No.21503149)the Program for Innovative Research Team in University of Tianjin(No.TD13-5074)the Project of Hubei University of Arts and Science(Nos.xk2020043,xk2020044,2020kypyfy015)。
文摘Photocatalytic water splitting utilizing solar energy is considered as one of the most ideal strategies for solving the ene rgy and environmental issues.Recently,two-dimensional(2 D)materials with an intrinsic dipole show great chance to achieve excellent photocatalytic performance.In this work,blue-phase monolayer carbon monochalcogenides(CX,X=S,Se)are constructed and systematically studied as photocatalysts for water splitting by performing first-principles calculations based on density functional theory.After confirming the great dynamical,thermal,and mechanical stability of CX monolayers,we observe that they possess moderate band gaps(2.41 eV for CS and 2.46 eV for CSe)and high carrier mobility(3.23×10^(4)cm^(2)V^(^(-1))s^(-1)for CS and 4.27×10^(3)cm^(2)V^(-1)s^(-1)for CSe),comparable to those of many recently reported 2 D photocatalysts.Moreover,these two monolayer materials are found to have large intrinsic dipole(0.43 D for CS and 0.51 D for CSe),thus the build-in internal electric field can be selfintroduced,which can effectively drive the separation of photongenerated carriers.More importantly,the well-aligned band edge as well as rather pronounced optical absorption in the visible-light and ultraviolet regions further ensure that our proposed CX monolayers can be used as high efficient photocatalysts for water splitting.Additionally,the effects of external strain on the electronic,optical and photocatalytic properties of CX monolayers are also evaluated.These theoretical predictions will stimulate further work to open up the energy-related applications of CX monolayers.
基金Project supported by the National Key R&D Program of China (Grant No.2018YFA0305800)the National Natural Science Foundation of China (Grant Nos.61925111,61888102,and 52102193)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences (Grant Nos.XDB28000000 and XDB30000000)CAS Project for Young Scientists in Basic Research (Grant No.YSBR-003)the Fundamental Research Funds for the Central Universities。
文摘Two-dimensional honeycomb lattices show great potential in the realization of Dirac nodal line fermions(DNLFs).Here,we successfully synthesized a gold telluride(AuTe)monolayer by direct tellurizing an Au(111)substrate.Low energy electron diffraction measurements reveal that it is(2×2)AuTe layer stacked onto(3×3)Au(111)substrate.Moreover,scanning tunneling microscopy images show that the AuTe layer has a honeycomb structure.Scanning transmission electron microscopy reveals that it is a single-atom layer.In addition,first-principles calculations demonstrate that the honeycomb AuTe monolayer exhibits Dirac nodal line features protected by mirror symmetry,which is validated by angle-resolved photoemission spectra.Our results establish that monolayer AuTe can be a good candidate to investigate 2D DNLFs and provides opportunities to realize high-speed low-dissipation devices.
文摘GroupqV monochalcogenides are emerging as a new class of layered materials beyond graphene, transition metal dichalcogenides （TMDCs）, and black phosphorus （BP）. In this paper, we report experimental and theoretical investigations of the band structure and transport properties of GeSe and its heterostructures. We find that GeSe exhibits a markedly anisotropic electronic transport, with maximum conductance along the armchair direction. Density functional theory calculations reveal that the effective mass is 2.7 times larger along the zigzag direction than the armchair direction; this mass anisotropy explains the observed anisotropic conductance. The crystallographic orientation of GeSe is confirmed by angle- resolved polarized Raman measurements, which are further supported by calculated Raman tensors for the orthorhombic structure. Novel GeSeflVIoS2 p-n heterojunctions are fabricated, combining the natural p-type doping in GeSe and n-type doping in MoS2. The temperature dependence of the measured junction current reveals that GeSe and MoS2 have a type-II band alignment with a conduction band offset of N 0.234 eV. The anisotropic conductance of GeSe may enable the development of new electronic and optoelectronic devices, such as high-efficiency thermoelectric devices and plasmonic devices with resonance frequency continuously tunable through light polarization direction. The unique GeSe/MoS2 p-n junctions with type-II alignment may become essential building blocks of vertical tunneling field-effect transistors for low-power applications. The novel p-type layered material GeSe can also be combined with n-type TMDCs to form heterogeneous complementary metal oxide semiconductor （CMOS） circuits.
