Two-dimensional(2D)moirésuperlattices have emerged as a versatile platform for uncovering exotic quantum phases,many of which arise in bilayer systems exhibiting Archimedean tessellation patterns such as triangul...Two-dimensional(2D)moirésuperlattices have emerged as a versatile platform for uncovering exotic quantum phases,many of which arise in bilayer systems exhibiting Archimedean tessellation patterns such as triangular,hexagonal,and kagome lattices.Here,we propose a strategy to engineer semiregular tessellation patterns in untwisted bilayer graphene by applying anisotropic epitaxial tensile strain(AETS)along crystallographic directions.Through force-field and firstprinciples calculations,we demonstrate that AETS can induce a rich variety of semiregular tessellation geometries,including truncated hextille,prismatic pentagon,and brick-phase arrangements.Characteristic electronic Dirac and flat bands of the lattice models associated with these semiregular tessellations are observed near the Fermi level,arising from interlayer interactions generated by the spatial rearrangement of AB,BA,and SP domains.Furthermore,the real-space observations of electronic kagome,distorted Lieb,brick-like,and one-dimensional stripe lattices demonstrate that AETS enables tunable semiregular tessellation lattices.Our study identifies AETS as a promising new degree of freedom in moiréengineering,offering a reproducible and scalable platform for exploring exotic electronic lattices in moirésystems.展开更多
Hafnia-based ferroelectric materials,like Hf_(0.5)Zr_(0.5)O_(2)(HZO),have received tremendous attention owing to their potentials for building ultra-thin ferroelectric devices.The orthorhombic(O)-phase of HZO is ferro...Hafnia-based ferroelectric materials,like Hf_(0.5)Zr_(0.5)O_(2)(HZO),have received tremendous attention owing to their potentials for building ultra-thin ferroelectric devices.The orthorhombic(O)-phase of HZO is ferroelectric but metastable in its bulk form under ambient conditions,which poses a considerable challenge to maintaining the operation performance of HZO-based ferroelectric devices.Here,we theoretically addressed this issue that provides parameter spaces for stabilizing the O-phase of HZO thin-films under various conditions.Three mechanisms were found to be capable of lowering the relative energy of the O-phase,namely,more significant surface-bulk portion of(111)surfaces,compressive c-axis strain,and positive electric fields.Considering these mechanisms,we plotted two ternary phase diagrams for HZO thin-films where the strain was applied along the in-plane uniaxial and biaxial,respectively.These diagrams indicate the O-phase could be stabilized by solely shrinking the film-thickness below 12.26 nm,ascribed to its lower surface energies.All these results shed considerable light on designing more robust and higher-performance ferroelectric devices.展开更多
At least four two-or quasi-one-dimensional allotropes and a mixture of them were theoretically predicted or experimentally observed for low-dimensional Te,namely theα,β,γ,δ,and chiral-α+δphases.Among them theγ...At least four two-or quasi-one-dimensional allotropes and a mixture of them were theoretically predicted or experimentally observed for low-dimensional Te,namely theα,β,γ,δ,and chiral-α+δphases.Among them theγandαphases were found to be the most stable phases for monolayer and thicker layers,respectively.Here,we found two novel low-dimensional phases,namely theεandζphases.Theζphase is over 29 meV/Te more stable than the most stable monolayerγphase,and theεphase shows comparable stability with the most stable monolayerγphase.The energetic difference between theζandαphases reduces with respect to the increased layer thickness and vanishes at the four-layer(12-sublayer)thickness,while this thickness increases under change doping.Bothεandζphases are metallic chains and layers,respectively.Theζphase,with very strong interlayer coupling,shows quantum well states in its layer-dependent bandstructures.These results provide significantly insight into the understanding of polytypism in Te few-layers and may boost tremendous studies on properties of various few-layer phases.展开更多
We carry out ab initio density functional theory calculations to study manipulation of electronic structures of selfassembled molecular nanostructures on metal surfaces by investigating the geometric and electronic pr...We carry out ab initio density functional theory calculations to study manipulation of electronic structures of selfassembled molecular nanostructures on metal surfaces by investigating the geometric and electronic properties of glycine molecules on Cu(100).It is shown that a glycine monolayer on Cu(100)forms a two-dimensional hydrogen-bonding network between the carboxyl and amino groups of glycine using a first principles atomistic calculation on the basis of a recently found structure.This network includes at least two hydrogen-bonding chains oriented roughly perpendicular to each other.Through molecule–metal electronic hybridization,these two chains selectively hybridized with the two isotropic degenerate Cu(100)surface states,leading to two anisotropic quasi-one-dimensional surface states.Electrons occupying these two states can near-freely move from a molecule to its adjacent molecules directly through the intermolecular hydrogen bonds,rather than mediated by the substrate.This results in the experimentally observed anisotropic free-electron-like behavior.Our results suggest that hydrogen-bonding chains are likely candidates for charge conductors.展开更多
Two-dimensional magnets have received increasing attention since Cr_2Ge_2Te_6 and CrI_3 were experimentally exfoliated and measured in 2017. Although layered ferromagnetic metals were demonstrated at room temperature,...Two-dimensional magnets have received increasing attention since Cr_2Ge_2Te_6 and CrI_3 were experimentally exfoliated and measured in 2017. Although layered ferromagnetic metals were demonstrated at room temperature, a layered ferromagnetic semiconductor with high Curie temperature(Tc) is yet to be unveiled. Here, we theoretically predicted a family of high Tcferromagnetic monolayers, namely MnNX and CrCX(X = Cl, Br and I; C = S, Se and Te). Their Tcvalues were predicted from over 100 K to near 500 K with Monte Carlo simulations using an anisotropic Heisenberg model. Eight members among them show semiconducting bandgaps varying from roughly 0.23 to 1.85 eV. These semiconducting monolayers also show extremely large anisotropy, i.e. ～10~1 for effective masses and ～10~2 for carrier mobilities, along the two in-plane lattice directions of these layers. Additional orbital anisotropy leads to a spin-locked linear dichroism, in different from previously known circular and linear dichroisms in layered materials.Together with the mobility anisotropy, it offers a spin-, dichroism-and mobility-anisotropy locking.These results manifest the potential of this 2D family for both fundamental research and high performance spin-dependent electronic and optoelectronic devices.展开更多
Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanc...Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons,tunable electronic structures and optical properties,and other superior advantages to these inorganic HJs.Here,we report a direct probe of the interfacial electronic structures of a crystalline monolayer(ML)perylene-3,4,9,10-tetracarboxylic-dianhydride(PTCDA)/ML-WSe_(2) HJ using scanning tunneling microscopy,photoluminescence,and first-principle calculations.Strong PTCDAAA/Se_(2) interfacial interactions lead to appreciable hybridization of the WSe_(2) conduction band with PTCDA unoccupied states,accompanying with a significant amount of PTCDA-to-WSe_(2) charge transfer(by 0.06 e/PTCDA).A type-ll band alignment was directly determined with a valence band offset of-1.69 eV,and an apparent conduction band offset of-1.57 eV.Moreover,we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.展开更多
基金supported by the National Natural Science Foundation of China(Grant Nos.52461160327,92477205,12474173,and 12104313)the National Key R&D Program of China(Grant No.2023YFA1406500)+3 种基金the Department of Science and Technology of Guangdong Province(Grant No.2021QN02L820)Shenzhen Science and Technology Program(Grant No.RCYX20231211090126026,the Stable Support Plan Program 20220810161616001)the Fundamental Research Funds for the Central Universitiesthe Research Funds of Renmin University of China(Grant No.22XNKJ30)。
文摘Two-dimensional(2D)moirésuperlattices have emerged as a versatile platform for uncovering exotic quantum phases,many of which arise in bilayer systems exhibiting Archimedean tessellation patterns such as triangular,hexagonal,and kagome lattices.Here,we propose a strategy to engineer semiregular tessellation patterns in untwisted bilayer graphene by applying anisotropic epitaxial tensile strain(AETS)along crystallographic directions.Through force-field and firstprinciples calculations,we demonstrate that AETS can induce a rich variety of semiregular tessellation geometries,including truncated hextille,prismatic pentagon,and brick-phase arrangements.Characteristic electronic Dirac and flat bands of the lattice models associated with these semiregular tessellations are observed near the Fermi level,arising from interlayer interactions generated by the spatial rearrangement of AB,BA,and SP domains.Furthermore,the real-space observations of electronic kagome,distorted Lieb,brick-like,and one-dimensional stripe lattices demonstrate that AETS enables tunable semiregular tessellation lattices.Our study identifies AETS as a promising new degree of freedom in moiréengineering,offering a reproducible and scalable platform for exploring exotic electronic lattices in moirésystems.
基金the Fund from the Ministry of Science and Technology(MOST)of China(Grant No.2018YFE0202700)the National Natural Science Foundation of China(Grant Nos.11974422 and 12104504)+2 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB30000000)the Fundamental Research Funds for the Central Universitiesthe Research Funds of Renmin University of China(Grant No.22XNKJ30)。
文摘Hafnia-based ferroelectric materials,like Hf_(0.5)Zr_(0.5)O_(2)(HZO),have received tremendous attention owing to their potentials for building ultra-thin ferroelectric devices.The orthorhombic(O)-phase of HZO is ferroelectric but metastable in its bulk form under ambient conditions,which poses a considerable challenge to maintaining the operation performance of HZO-based ferroelectric devices.Here,we theoretically addressed this issue that provides parameter spaces for stabilizing the O-phase of HZO thin-films under various conditions.Three mechanisms were found to be capable of lowering the relative energy of the O-phase,namely,more significant surface-bulk portion of(111)surfaces,compressive c-axis strain,and positive electric fields.Considering these mechanisms,we plotted two ternary phase diagrams for HZO thin-films where the strain was applied along the in-plane uniaxial and biaxial,respectively.These diagrams indicate the O-phase could be stabilized by solely shrinking the film-thickness below 12.26 nm,ascribed to its lower surface energies.All these results shed considerable light on designing more robust and higher-performance ferroelectric devices.
基金Project supported by the Science Fund from the Ministry of Science and Technology(MOST)of China(Grant No.2018YFE0202700)the National Natural Science Foundation of China(Grant Nos.11274380,91433103,11622437,61674171,11974422,and 61761166009)+3 种基金the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB30000000)the Fundamental Research Funds for the Central Universities of China and the Research Funds of Renmin University of China(Grant No.16XNLQ01)the Research Grant No.Council of Hong Kong,China(Grant No.N_PolyU540/17)the Hong Kong Polytechnic University(Grant No.G-SB53).Cong Wang was supported by the Outstanding Innovative Talents Cultivation Funded Programs 2017 of Renmin University of China.
文摘At least four two-or quasi-one-dimensional allotropes and a mixture of them were theoretically predicted or experimentally observed for low-dimensional Te,namely theα,β,γ,δ,and chiral-α+δphases.Among them theγandαphases were found to be the most stable phases for monolayer and thicker layers,respectively.Here,we found two novel low-dimensional phases,namely theεandζphases.Theζphase is over 29 meV/Te more stable than the most stable monolayerγphase,and theεphase shows comparable stability with the most stable monolayerγphase.The energetic difference between theζandαphases reduces with respect to the increased layer thickness and vanishes at the four-layer(12-sublayer)thickness,while this thickness increases under change doping.Bothεandζphases are metallic chains and layers,respectively.Theζphase,with very strong interlayer coupling,shows quantum well states in its layer-dependent bandstructures.These results provide significantly insight into the understanding of polytypism in Te few-layers and may boost tremendous studies on properties of various few-layer phases.
基金Supported by the National Natural Science Foundation of China(Grant Nos.11622437,11804247,61674171,and 11974422)the Fundamental Research Funds for the Central Universities of China+1 种基金the Research Funds of Renmin University of China(Grant Nos.19XNQ025 and 19XNH066)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB30000000)。
文摘We carry out ab initio density functional theory calculations to study manipulation of electronic structures of selfassembled molecular nanostructures on metal surfaces by investigating the geometric and electronic properties of glycine molecules on Cu(100).It is shown that a glycine monolayer on Cu(100)forms a two-dimensional hydrogen-bonding network between the carboxyl and amino groups of glycine using a first principles atomistic calculation on the basis of a recently found structure.This network includes at least two hydrogen-bonding chains oriented roughly perpendicular to each other.Through molecule–metal electronic hybridization,these two chains selectively hybridized with the two isotropic degenerate Cu(100)surface states,leading to two anisotropic quasi-one-dimensional surface states.Electrons occupying these two states can near-freely move from a molecule to its adjacent molecules directly through the intermolecular hydrogen bonds,rather than mediated by the substrate.This results in the experimentally observed anisotropic free-electron-like behavior.Our results suggest that hydrogen-bonding chains are likely candidates for charge conductors.
基金supported by the National Natural Science Foundation of China(11274380,91433103,11622437 and 61674171)the Fundamental Research Funds for the Central Universities of China+2 种基金the Research Funds of Renmin University of China(16XNLQ01)the Strategic Priority Research Program of Chinese Academy of Sciences(XDB30000000)supported by the Outstanding Innovative Talents Cultivation Funded Programs 2017 of Renmin University of China
文摘Two-dimensional magnets have received increasing attention since Cr_2Ge_2Te_6 and CrI_3 were experimentally exfoliated and measured in 2017. Although layered ferromagnetic metals were demonstrated at room temperature, a layered ferromagnetic semiconductor with high Curie temperature(Tc) is yet to be unveiled. Here, we theoretically predicted a family of high Tcferromagnetic monolayers, namely MnNX and CrCX(X = Cl, Br and I; C = S, Se and Te). Their Tcvalues were predicted from over 100 K to near 500 K with Monte Carlo simulations using an anisotropic Heisenberg model. Eight members among them show semiconducting bandgaps varying from roughly 0.23 to 1.85 eV. These semiconducting monolayers also show extremely large anisotropy, i.e. ～10~1 for effective masses and ～10~2 for carrier mobilities, along the two in-plane lattice directions of these layers. Additional orbital anisotropy leads to a spin-locked linear dichroism, in different from previously known circular and linear dichroisms in layered materials.Together with the mobility anisotropy, it offers a spin-, dichroism-and mobility-anisotropy locking.These results manifest the potential of this 2D family for both fundamental research and high performance spin-dependent electronic and optoelectronic devices.
基金supported by the National Key R&D Program of China(Nos.2018FYA0305800 and 2018YFA0703700)the National Natural Science Foundation of China(Nos.11774268 and 11974012)+2 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(No.XDB30000000)support from the Fundamental Research Funds for the Central Universities,Chinathe Research Funds of Renmin University of China(Nos.16XNLQ01 and 19XNQ025)。
文摘Semiconducting heterojunctions(HJs),comprised of atomically thin transition metal dichalcogenides(TMDs),have shown great potentials in electronic and optoelectronic applications.Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons,tunable electronic structures and optical properties,and other superior advantages to these inorganic HJs.Here,we report a direct probe of the interfacial electronic structures of a crystalline monolayer(ML)perylene-3,4,9,10-tetracarboxylic-dianhydride(PTCDA)/ML-WSe_(2) HJ using scanning tunneling microscopy,photoluminescence,and first-principle calculations.Strong PTCDAAA/Se_(2) interfacial interactions lead to appreciable hybridization of the WSe_(2) conduction band with PTCDA unoccupied states,accompanying with a significant amount of PTCDA-to-WSe_(2) charge transfer(by 0.06 e/PTCDA).A type-ll band alignment was directly determined with a valence band offset of-1.69 eV,and an apparent conduction band offset of-1.57 eV.Moreover,we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.
