Two-dimensional(2D)semiconductors have emerged as promising candidates in next-generation nanoelectronics and sustainable energy technologies,particularly in photoelectrochemical water splitting,due to their exception...Two-dimensional(2D)semiconductors have emerged as promising candidates in next-generation nanoelectronics and sustainable energy technologies,particularly in photoelectrochemical water splitting,due to their exceptional quantum confinement effects and tunable optoelectronic properties.Accurate determination of electronic band gaps remains a critical prerequisite for rational material design in advanced optoelectronic applications.However,the commonly used density functional theory approach with conventional functionals suffers from intrinsic deficiencies in predicting semiconductor band gaps,while calculations with higher hierarchy of functionals like the HSE06 hybrid functional or based on higher level methodologies such as GW approximation incur prohibitive computational costs.To address this challenge,here we propose a reference-guided graph neural network(RG-GNN)framework that achieves HSE06-level accuracy through efficient machine learning.Our approach uniquely embeds an input reference value for the target property with minimal elementary descriptors encoding the structural information of the materials in the model,enabling high-accuracy band gap prediction at the HSE06 level.The model achieves a mean absolute error of 0.15 eV on unseen 2D semiconductor systems compared to HSE06 band gaps.Systematic ablation studies reveal that the reference-guided mechanism reduces prediction error by 83.3%and significantly decreases training dataset requirements for model convergence compared to conventional GNN architectures.Our results demonstrates that topological atomic descriptors from primitive cells,when combined with appropriate reference values,contain sufficient information for highly accurate band gap prediction in 2D materials.展开更多
We calculate the electronic properties and carrier mobility of perovskite CH3NH3SnI3as a solar cell absorber by using the hybrid functional method. The calculated result shows that the electron and hole mobilities hav...We calculate the electronic properties and carrier mobility of perovskite CH3NH3SnI3as a solar cell absorber by using the hybrid functional method. The calculated result shows that the electron and hole mobilities have anisotropies with a large magnitude of 1.4 × 104cm2·V-1·s-1along the y direction. In view of the huge difference between hole and electron mobilities, the perovskite CH3NH3 Sn I3can be considered as a p-type semiconductor. We also discover a relationship between the effective mass anisotropy and electronic occupation anisotropy. The above results can provide reliable guidance for its experimental applications in electronics and optoelectronics.展开更多
III-V semiconductors such as GaAs are widely studied as promising candidates for high-speed integrated circuit.Despite these applications for conventional bulk structures,their fundamental physical properties in the n...III-V semiconductors such as GaAs are widely studied as promising candidates for high-speed integrated circuit.Despite these applications for conventional bulk structures,their fundamental physical properties in the nanoscale limit are still in scarcity,which is of great importance for the development of nanoelectronics.In this work,we demonstrate that the III-V semiconductor MX(M=Al,Ga,In;X=P,As,Sb)in its two-dimensional(2D)limit could exhibit double layer honeycomb(DLHC)configuration and distorted tetrahedral coordination,according to our first-principles calculations with HSE06 hybrid functional.It is found that surface reconstruction endows 2D III-V DLHCs with pronouncedly different electronic and magnetic properties from their bulk counterparts due to strong interlayer coupling.Mexican-hat-shape bands emerge at the top valence bands of pristine AlP,GaP,InP,AlAs,and InAs DLHCs,inducing the density of states showing a sharp van Hove singularity near the Fermi level.As a result,these DLHCs exhibit itinerant magnetism upon moderate hole doping,while the rest GaAs,AlSb,GaSb,and InSb DLHCs become magnetic under tensile strain with hole doping.With an exchange splitting of the localized pz states at the top valence bands,the hole-doped III-V DLHCs become half-metals with 100%spin-polarization.Remarkably,the InSb DLHC shows inverted band structure near the Fermi level,bringing about nontrivial topological band structures in stacked InSb DLHC due to the strong spin-orbital coupling.These III-V DLHCs expand the members of 2D material family and their exotic magnetic and topological properties may offer great potential for applications in the novel electronic and spintronic devices.展开更多
The electronic band structures and band gap bowing parameters of In_xGa_（1-x）N are studied by the firstprinciples method based on the density functional theory. Calculations by employing both the Heyd-ScuseriaErnzer...The electronic band structures and band gap bowing parameters of In_xGa_（1-x）N are studied by the firstprinciples method based on the density functional theory. Calculations by employing both the Heyd-ScuseriaErnzerh of hybrid functional（HSE06） and the Perdew-Burke-Ernzerhof（PBE） one are performed. We found that the theoretical band gap bowing parameter is dependent significantly on the calculation method, especially on the exchange-correlation functional employed in the DFT calculations. The band gap of In_xGa_（1-x）N alloy decreases considerably when the In constituent x increases. It is the interactions of s–s and p–p orbitals between anions and cations that play significant roles in formatting the band gaps bowing. In general, the HSE06 hybrid functional could provide a good alternative to the PBE functional in calculating the band gap bowing parameters.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.22173052)。
文摘Two-dimensional(2D)semiconductors have emerged as promising candidates in next-generation nanoelectronics and sustainable energy technologies,particularly in photoelectrochemical water splitting,due to their exceptional quantum confinement effects and tunable optoelectronic properties.Accurate determination of electronic band gaps remains a critical prerequisite for rational material design in advanced optoelectronic applications.However,the commonly used density functional theory approach with conventional functionals suffers from intrinsic deficiencies in predicting semiconductor band gaps,while calculations with higher hierarchy of functionals like the HSE06 hybrid functional or based on higher level methodologies such as GW approximation incur prohibitive computational costs.To address this challenge,here we propose a reference-guided graph neural network(RG-GNN)framework that achieves HSE06-level accuracy through efficient machine learning.Our approach uniquely embeds an input reference value for the target property with minimal elementary descriptors encoding the structural information of the materials in the model,enabling high-accuracy band gap prediction at the HSE06 level.The model achieves a mean absolute error of 0.15 eV on unseen 2D semiconductor systems compared to HSE06 band gaps.Systematic ablation studies reveal that the reference-guided mechanism reduces prediction error by 83.3%and significantly decreases training dataset requirements for model convergence compared to conventional GNN architectures.Our results demonstrates that topological atomic descriptors from primitive cells,when combined with appropriate reference values,contain sufficient information for highly accurate band gap prediction in 2D materials.
基金supported by the National Natural Science Foundation of China(Grant No.51172067)the Hunan Provincial Natural Science Fund for Distinguished Young Scholars,China(Grant No.13JJ1013)+1 种基金the Specialized Research Fund for the Doctoral Program of Higher Education,China(Grant No.20130161110036)the New Century Excellent Talents in University,China(Grant No.NCET-12-0171.D)
文摘We calculate the electronic properties and carrier mobility of perovskite CH3NH3SnI3as a solar cell absorber by using the hybrid functional method. The calculated result shows that the electron and hole mobilities have anisotropies with a large magnitude of 1.4 × 104cm2·V-1·s-1along the y direction. In view of the huge difference between hole and electron mobilities, the perovskite CH3NH3 Sn I3can be considered as a p-type semiconductor. We also discover a relationship between the effective mass anisotropy and electronic occupation anisotropy. The above results can provide reliable guidance for its experimental applications in electronics and optoelectronics.
基金sponsored by the National Natural Science Foundation of China(21706195,51462030)the Research Fund for the Doctoral Program of Tongren University(trxyDH1510)+1 种基金the Science and Technology Program of Guizhou Province(QKHJC2016-1149)the Guizhou Provincial Dep
基金supported by the National Natural Science Foundation of China(Nos.12274335 and 52202111)the Natural Science Foundation of Shaanxi Province(Nos.2022JM-008,2021JC-062,and 2019TD-020)This research used the resources of the HPCC platform in Xi’an Jiaotong University.
文摘III-V semiconductors such as GaAs are widely studied as promising candidates for high-speed integrated circuit.Despite these applications for conventional bulk structures,their fundamental physical properties in the nanoscale limit are still in scarcity,which is of great importance for the development of nanoelectronics.In this work,we demonstrate that the III-V semiconductor MX(M=Al,Ga,In;X=P,As,Sb)in its two-dimensional(2D)limit could exhibit double layer honeycomb(DLHC)configuration and distorted tetrahedral coordination,according to our first-principles calculations with HSE06 hybrid functional.It is found that surface reconstruction endows 2D III-V DLHCs with pronouncedly different electronic and magnetic properties from their bulk counterparts due to strong interlayer coupling.Mexican-hat-shape bands emerge at the top valence bands of pristine AlP,GaP,InP,AlAs,and InAs DLHCs,inducing the density of states showing a sharp van Hove singularity near the Fermi level.As a result,these DLHCs exhibit itinerant magnetism upon moderate hole doping,while the rest GaAs,AlSb,GaSb,and InSb DLHCs become magnetic under tensile strain with hole doping.With an exchange splitting of the localized pz states at the top valence bands,the hole-doped III-V DLHCs become half-metals with 100%spin-polarization.Remarkably,the InSb DLHC shows inverted band structure near the Fermi level,bringing about nontrivial topological band structures in stacked InSb DLHC due to the strong spin-orbital coupling.These III-V DLHCs expand the members of 2D material family and their exotic magnetic and topological properties may offer great potential for applications in the novel electronic and spintronic devices.
基金Project supported by the National Natural Science Foundation of China(Nos.11204257,21233004)the China Postdoctoral Science Foundation(No.2012M511447)
文摘The electronic band structures and band gap bowing parameters of In_xGa_（1-x）N are studied by the firstprinciples method based on the density functional theory. Calculations by employing both the Heyd-ScuseriaErnzerh of hybrid functional（HSE06） and the Perdew-Burke-Ernzerhof（PBE） one are performed. We found that the theoretical band gap bowing parameter is dependent significantly on the calculation method, especially on the exchange-correlation functional employed in the DFT calculations. The band gap of In_xGa_（1-x）N alloy decreases considerably when the In constituent x increases. It is the interactions of s–s and p–p orbitals between anions and cations that play significant roles in formatting the band gaps bowing. In general, the HSE06 hybrid functional could provide a good alternative to the PBE functional in calculating the band gap bowing parameters.
