Heat dissipation and thermal switches are vital for adaptive cooling and extending the lifespan of electronic devices and batteries. In this work, we conducted high-throughput investigations on the thermal transport o...Heat dissipation and thermal switches are vital for adaptive cooling and extending the lifespan of electronic devices and batteries. In this work, we conducted high-throughput investigations on the thermal transport of 24 experimentally realized two-dimensional(2D) materials and their potential as thermal switches, leveraging machine-learning-assisted strain engineering and phonon transport simulations. We identified several highperformance thermal switches with ratios exceeding 2, with germanene(Ge) achieving an ultrahigh ratio of up to9.64 within the reversible deformation range. The underlying mechanism is strain-induced bond softening, which sensitively affects anharmonicity represented by three-and four-phonon scattering. The widespread occurrence of four-phonon scattering was confirmed in the thermal transport of 2D materials. Opposite switching trends were discovered, with 2D transition metal dichalcogenide materials showing negative responses to tensile strain while buckled 2D elemental materials showed positive responses. We further proposed a screening descriptor based on strain-induced changes in the Gr¨uneisen parameter for efficiently identifying new high-performance thermal switch materials. This work establishes a paradigm for thermal energy control in 2D materials through strain engineering, which may be experimentally realized in the future via bending, substrate mismatch, and related approaches, thereby laying a robust foundation for further developments and applications.展开更多
The precise control of wrinkles and strain gradients in nanofilm is of significant interest due to their profound influence on electronic band structures and spin states.Here,we employ ultrafast electron diffraction(U...The precise control of wrinkles and strain gradients in nanofilm is of significant interest due to their profound influence on electronic band structures and spin states.Here,we employ ultrafast electron diffraction(UED)to study the picosecond-scale dynamics of laser-induced bending in 2H-MoTe2 thin films.展开更多
CONSPECTUS:Two-dimensional(2D)materials form a large and diverse family of materials with extremely rich compositions,ranging from graphene to complex transition metal derivatives.They exhibit unique physical,chemical...CONSPECTUS:Two-dimensional(2D)materials form a large and diverse family of materials with extremely rich compositions,ranging from graphene to complex transition metal derivatives.They exhibit unique physical,chemical,and electronic properties,making 2D materials highly promising in the fields of sustainable energy storage and electrocatalysis.Although significant progress has been made in the design and performance optimization of 2D materials,challenges persist,particularly in energy storage and electrocatalysis.A key issue is the restacking or aggregation of these materials in the powder form,which hinders ion transport and reduces their overall performance by limiting the effective surface area.展开更多
With the rapidly increasing amount of materials data being generated in a variety of projects,efficient and accurate classification of atomistic structures is essential.A current barrier to effective database queries ...With the rapidly increasing amount of materials data being generated in a variety of projects,efficient and accurate classification of atomistic structures is essential.A current barrier to effective database queries lies in the often ambiguous,inconsistent,or completely missing classification of existing data,highlighting the need for standardized,automated,and verifiable classification methods.This work proposes a robust solution for identifying and classifying a wide spectrum of materials through an iterative technique,called symmetry-based clustering(SBC).Because SBC is not a machine learningbased method,it requires no prior training.Instead,it identifies clusters in atomistic systems by automatically recognizing common unit cells.We demonstrate the potential of SBC to provide automated,reliable classification and to reveal well-known symmetry properties of various materials.Even noisy systems are shown to be classifiable,showing the suitability of our algorithm for real-world data applications.The software implementation is provided in the open-source Python package,MatID,exploiting synergies with popular atomic-structure manipulation libraries and extending the accessibility of those libraries through the NOMAD platform.展开更多
Understanding the interplay between screening,electronic correlations,and collective excitations is essential for the design of two-dimensional quantum materials.Here,we present a comprehensive first-principles study ...Understanding the interplay between screening,electronic correlations,and collective excitations is essential for the design of two-dimensional quantum materials.Here,we present a comprehensive first-principles study of more than 60 MA_(2)Z_(4)monolayers,encompassing semiconducting,metallic,cold-metallic,magnetic,and topological phases.Using the constrained random phase approximation(cRPA),wecompute material-specific effectiveCoulomb interaction parametersU,U0,and J,including their spatial dependence across distinct correlated subspaces defined by local coordination and crystal symmetry.In semiconducting compounds,long-range nonlocal interactions persist,revealing unconventional screening and suggesting strong excitonic effects beyond simple dielectricmodels.In cold-metallic systems,sizable long-range Coulomb interactions remain despite the presence of free carriers,highlighting their atypical metallic screening.Among 33-valence-electron compounds,we find U^(eff)>W in theβ2 phase,indicating proximity to charge-density-wave or Mott instabilities.Several V-and Nb-based systems exhibit intermediate-to-strong correlation strength,with U/W>1 in multiple cases.Using cRPA-derived Stoner parameters,we identify magnetic instabilities in various V-,Nb-,Cr-,andMn-based compounds.Finally,selected cold-metallic systems display plasmon dispersions that deviate from the conventional√q behavior,revealing nearly non-dispersive low-energy modes.These results position MA_(2)Z_(4)monolayers as a versatile platform for investigating correlation-driven instabilities and emergent collective behavior in two dimensions.展开更多
Two-dimensional(2D)materials attract considerable attention due to their remarkable electronic,mechanical and optical properties.Despite their use in combination with substrates in practical applications,computational...Two-dimensional(2D)materials attract considerable attention due to their remarkable electronic,mechanical and optical properties.Despite their use in combination with substrates in practical applications,computational studies often neglect the effects of substrate interactions for simplicity.This study presents a novel method for predicting the atomic structure of 2D materials on substrates by combining an evolutionary algorithm,a lattice-matching technique,an automated machinelearning interatomic potentials training protocol,and the ab initio thermodynamics approach.Using the molybdenum-sulfur system on a sapphire substrate as a case study,we reveal several new stable and metastable structures,including previously known 1H-MoS_(2)and newly found Pmma Mo_(3)S_(2),P1^(-)Mo_(2)S,P2_(1)m Mo_(5)S_(3),and P_(4)mm Mo_(4)S,where the Mo_(4)S structure is specifically stabilized by interaction with the substrate.Finally,we use the ab initio thermodynamics approach to predict the synthesis conditions of the discovered structures in the parameter space of the commonly used chemical vapor deposition technique.展开更多
Transmission electron microscopy(TEM)is an indispensable tool for elucidating the intrinsic atomic structures of materials and provides deep insights into defect dynamics,phase transitions,and nanoscale structural det...Transmission electron microscopy(TEM)is an indispensable tool for elucidating the intrinsic atomic structures of materials and provides deep insights into defect dynamics,phase transitions,and nanoscale structural details.While numerous intriguing physical properties have been revealed in recently discovered two-dimensional(2D)quantummaterials,many exhibit significant sensitivity towater and oxygen under ambient conditions.This inherent instability complicates sample preparation for TEM analysis and hinders accurate property measurements.This review highlights recent technical advancements to preserve the intrinsic structures of water-and oxygen-sensitive 2D materials for atomic-scale characterizations.A critical development discussed in this review is implementing an inert gas-protected glovebox integrated system(GIS)designed specifically for TEM experiments.In addition,this review emphasizes air-sensitivematerials such as 2D transitionmetal dichalcogenides,transition metal dihalides and trihalides,and low-dimensional magnetic materials,demonstrating breakthroughs in overcoming their environmental sensitivity.Furthermore,the progress in TEM characterization enabled by the GIS is analyzed to provide a comprehensive overview of state-of-the-art methodologies in this rapidly advancing field.展开更多
The design of spin-orbit torque properties in two-dimensional(2D)materials presents one of the challenges of modern spintronics.In this context,2D layers involving rare-earth ions−which give rise to robust magnetism,e...The design of spin-orbit torque properties in two-dimensional(2D)materials presents one of the challenges of modern spintronics.In this context,2D layers involving rare-earth ions−which give rise to robust magnetism,exhibit pronounced orbital polarization of the states,and carry strong spin-orbit interaction—hold particular promise.Here,we investigate ferromagnetic Janus H-phase monolayers of 4f-Eu rare-earth dichalcogenides EuSP,EuSSe,and EuSCl using first-principles calculations.We demonstrate that all compounds exhibit significant spin-orbit torques which originate predominantly in the colossal current-induced orbital response on the Eu f-electrons.Moreover,we demonstrate that the corresponding orbital torques can be used to drive strong in-plane currents of orbital angular momentum with non-trivial direction of orbital polarization,constituting the effect of in-plane orbital pumping.We provide an interpretation of this effect in terms of orbital-to-orbital-curent conversion,and draw a simple qualitative picture of orbital pumping by magnetization dynamics in two dimensional systems.Our findings promote f-orbital-based 2D materials as a promising platform for in-plane orbital pumping and spin-orbit torque applications,and motivate further research on educated design of orbital properties for orbitronics with 2D materials.展开更多
With the rapid advancement of the information age,the demand for multi-dimensional light information detection has significantly increased.Traditional Fourier-transform infrared(FTIR)spectrometers and pooptical power,...With the rapid advancement of the information age,the demand for multi-dimensional light information detection has significantly increased.Traditional Fourier-transform infrared(FTIR)spectrometers and pooptical power,andlarimeters,due to their bulky structure,are no longer suitable for emerging fields such as medical diagnostics,secure communications,and autonomous driving.As a result,there is a pressing need to develop new miniaturized on-chip devices.The abundant two-dimensional(2D)materials,with their unique light-matter interactions,offer the potential to construct high-dimensional spatial mappings of incident light,paving the way for the development of novel ultra-compact multi-dimensional deep optical sensing technologies.Here,we review the interconnections of multi-dimensional information and their relationship with 2D materials.We then focus on recent advances in the development of novel dimensional detectors based on 2D materials,covering dimensions such as intensity,time,space,polarization,phase angle,and wavelength.Furthermore,we discuss cutting-edge technologies in multi-dimensional fusion detection and highlight future technological prospects,with a particular emphasis on on-chip integration and future development.展开更多
Two-dimensional(2D)transition metal dichalcogenides(TMDs),which allow atomic-scale manipulation,have supe-rior electrical and optical properties that challenge the limits of traditional bulk semiconductors like silico...Two-dimensional(2D)transition metal dichalcogenides(TMDs),which allow atomic-scale manipulation,have supe-rior electrical and optical properties that challenge the limits of traditional bulk semiconductors like silicon^([1,2]).As a repre-sentative TMD and a promising 2D channel material for high-performance,scalable p-type transistors,tungsten diselenide(WSe_(2))has attracted considerable academic and industrial interest for its potential in advanced complementary metal−oxide−semiconductor(CMOS)logic technology and in extending Moore’s Law^([3−7]).展开更多
Dramatic fluorescence enhancement in two-dimensional(2D)van der Waals materials(vdWMs)coupled to plasmonic nanostructures has the potential to enable ultrathin,flexible,and high-brightness illumination devices.However...Dramatic fluorescence enhancement in two-dimensional(2D)van der Waals materials(vdWMs)coupled to plasmonic nanostructures has the potential to enable ultrathin,flexible,and high-brightness illumination devices.However,addressing the limitation of locally scattered small plasmon-enhanced areas remains challenging.Here,we present a 2D plasmonic enhancement of photoluminescence(PL)spanning nearly 800μm^(2),enabled by surface lattice resonance(SLR)in a 2D vdWM-Au slot lattice hybrid.The Au slot lattice is designed and fabricated using Babinet’s principle and Rayleigh’s anomaly to maximize radiative decay rate and induce non-local photo-excitation in a MoSe_(2)monolayer.For emitted PL coupled with SLR,enhanced by up to 32-fold,we investigate its in-plane directivity and long-range propagation using angle-and space-resolved spectroscopic PL measurements.Our experiment reveals that a nearly 800μm^(2)2D luminescent sheet can be achieved regardless of the size of the MoSe_(2)crystal,even with a sub-μm^(2)flake.This work provides a new type of ultrabright,large-area 2D luminescent material,suitable for a range of optical illumination,communication,and sensing devices.展开更多
Based on the nonlinear saturable absorption properties(NSAPs)of a two-dimensional(2D)material of antimony selenide(Sb_(2)Se_(3)),a Q-switched erbium-doped fiber(EDF)laser is systematically demonstrated.The Sb_(2)Se_(3...Based on the nonlinear saturable absorption properties(NSAPs)of a two-dimensional(2D)material of antimony selenide(Sb_(2)Se_(3)),a Q-switched erbium-doped fiber(EDF)laser is systematically demonstrated.The Sb_(2)Se_(3)nano sheets are prepared by liquid-phase exfoliation(LPE)method.After the sandwich-structured Sb_(2)Se_(3)saturable absorber(SA)is fabricated,the NSAPs are characterized and the modulation depth,the saturation intensity and the unsaturated loss are determined to be 25.2%,2.02 MW/cm^(2),and 3.29%,respectively.When the as-prepared Sb_(2)Se_(3)-SA is integrated into the ring cavity,the laser operates at a stable Q-switching regime in the pump power range of 100—400 mW.The laser oscillates at the central wavelength of 1558.48 nm with a 3 dB bandwidth of 2.32 nm.Take the advantages of the Sb_(2)Se_(3)-SA,the pulse duration can be compressed from 40.49 kHz to 128.12 kHz.At the pump power of 400 mW,the Q-switching laser gives the narrowest pulse duration the highest average output power,the largest pulse energy,and the signal-to-noise ratio(SNR)of 0.93μs,2.16 mW,16.89 nJ,and 53 dB,respectively.Our new attempt on Sb_(2)Se_(3)-based Q-switched EDF laser,combining the existing mode-locking achievements,proves that Sb_(2)Se_(3)is a powerful candidate for pulse compression due to the characteristics of high modulation depth and high stability.展开更多
Rechargeable lithium-sulfur(Li-S)batteries have attracted significant research attention due to their high capacity and energy density.However,their commercial applications are still hindered by challenges such as the...Rechargeable lithium-sulfur(Li-S)batteries have attracted significant research attention due to their high capacity and energy density.However,their commercial applications are still hindered by challenges such as the shuttle effect of soluble lithium sulfide species,the insulating nature of sulfur,and the fast capacity decay of the electrodes.Various efforts are devoted to address these problems through questing more conductive hosts with abundant polysulfide chemisorption sites,as well as modifying the separators to physically/chemically retard the polysulfides migration.Two dimensional transition metal carbides,carbonitrides and nitrides,so-called MXenes,are ideal for confining the polysulfides shuttling effects due to their high conductivity,layered structure as well as rich surface terminations.As such,MXenes have thus been widely studied in Li-S batteries,focusing on the conductive sulfur hosts,polysulfides interfaces,and separators.Therefore,in this review,we summarize the significant progresses regarding the design of multifunctional MXene-based Li-S batteries and discuss the solutions for improving electrochemical performances in detail.In addition,challenges and perspectives of MXenes for Li-S batteries are also outlined.展开更多
In this study,we have developed a high-sensitivity,near-infrared photodetector based on PdSe2/GaAs heterojunction,which was made by transferring a multilayered PdSe2 film onto a planar GaAs.The as-fabricated PdSe2/GaA...In this study,we have developed a high-sensitivity,near-infrared photodetector based on PdSe2/GaAs heterojunction,which was made by transferring a multilayered PdSe2 film onto a planar GaAs.The as-fabricated PdSe2/GaAs heterojunction device exhibited obvious photovoltaic behavior to 808 nm illumination,indicating that the near-infrared photodetector can be used as a self-driven device without external power supply.Further device analysis showed that the hybrid heterojunction exhibited a high on/off ratio of 1.16×10^5 measured at 808 nm under zero bias voltage.The responsivity and specific detectivity of photodetector were estimated to be 171.34 mA/W and 2.36×10^11 Jones,respectively.Moreover,the device showed excellent stability and reliable repeatability.After 2 months,the photoelectric characteristics of the near-infrared photodetector hardly degrade in air,attributable to the good stability of the PdSe2.Finally,the PdSe2/GaAs-based heterojunction device can also function as a near-infrared light sensor.展开更多
Two-dimensional（2 D） materials have attracted increasing attentions recently due to their unique physical and chemical properties. We herein report the synthesis of four chemically stable 2 D covalent organic nanosh...Two-dimensional（2 D） materials have attracted increasing attentions recently due to their unique physical and chemical properties. We herein report the synthesis of four chemically stable 2 D covalent organic nanosheets（CONs） with large lateral sizes（up to 200 mm） and high aspect ratios（〉20 000） at the air-water interface through the Langmuir-Blodgett method. These CONs exhibit good crystallinity proved by high resolution transmission electron microscopy（HRTEM） and selected area electron diffraction（SAED）. In addition, the hydrophobicity of these CONs can be systematically adjusted by the introduction of various functional groups, making them suitable as functional coating and membrane materials.展开更多
The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate interaction.By using in situ surface measurements,we demo...The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate interaction.By using in situ surface measurements,we demonstrate that the overlayer–substrate interaction can be tuned by doping near-surface Ar nanobubbles.The interfacial coupling strength significantly decreases with near-surface Ar nanobubbles,accompanying by an“anisotropic to isotropic”growth transformation.On the substrate containing near-surface Ar,the growth front crosses entire surface atomic steps in both uphill and downhill directions with no difference,and thus,the morphology of the two-dimensional(2D)overlayer exhibits a round-shape.Especially,the round-shaped 2D overlayers coalesce seamlessly with a growth acceleration in the approaching direction,which is barely observed in the synthesis of 2D materials.This can be attributed to the immigration lifetime and diffusion rate of growth species,which depends on the overlayer–substrate interaction and the surface catalysis.Furthermore,the“round to hexagon”morphological transition is achieved by etching-regrowth,revealing the inherent growth kinetics under quasi-freestanding conditions.These findings provide a novel promising way to modulate the growth,coalescence,and etching dynamics of 2D materials on solid surfaces by adjusting the strength of overlayer–substrate interaction,which contributes to optimization of large-scale production of 2D material crystals.展开更多
We conduct a systematic investigation of the role of Hubbard U corrections in electronic structure calculations of two-dimensional(2D)materials containing 3d transition metals.Specifically,we use density functional th...We conduct a systematic investigation of the role of Hubbard U corrections in electronic structure calculations of two-dimensional(2D)materials containing 3d transition metals.Specifically,we use density functional theory(DFT)with the PBE and PBE+U approximations to calculate the crystal structure,band gaps,and magnetic parameters of 638 monolayers.Based on a comprehensive comparison to experiments we first establish that the inclusion of the U correction worsens the accuracy for the lattice constants.Consequently,PBE structures are used for subsequent property evaluations.The band gaps show a significant dependence on U.In particular,for 134(21%)of the materials the U parameter induces a metal-to-insulator transition.For the magnetic materials we calculate the magnetic moment,magnetic exchange coupling,and magnetic anisotropy parameters.In contrast to the band gaps,the size of the magnetic moments shows only weak dependence on U.Both the exchange energies and magnetic anisotropy parameters are systematically reduced by theU correction.On this basis we conclude that the Hubbard U correction will lead to lower predicted Curie temperatures in 2D materials.All the calculated properties are available in the Computational 2D Materials Database(C2DB).展开更多
Hexagonal boron nitride nanosheets(HBNNSs)have huge potential in the field of coating materials owing to their remarkable chemical stability,mechanical strength and thermal conductivity.Thin-layer hBNNSs were obtained...Hexagonal boron nitride nanosheets(HBNNSs)have huge potential in the field of coating materials owing to their remarkable chemical stability,mechanical strength and thermal conductivity.Thin-layer hBNNSs were obtained by a liquid-phase exfoliation of h-BN powders and incorporated into EVA coatings for improving the safety performance of 1,3,5,7-tetranitro-1,3,5,7-tetrazocane(HMX).HBNNSs and ethylene-vinyl acetate copolymer(EVA)were introduced to HMX by a solvent-slurry process.For comparison,the HMX/EVA and HMX/EVA/graphene(HMX/EVA/G)composites were also prepared by a similar process.The morphology,crystal form,surface element distribution,thermal decomposition property and impact sensitivity of HMX/EVA/hBNNSs composites were contrastively investigated.Results showed that as prepared HMX/EVA/hBNNSs composites were well coated with hBNNSs and EVA,and exhibited better thermal stability and lower impact sensitivity than that of HMX/EVA and HMX/EVA/G composites,suggesting superior performance of desensitization of hBNNSs in explosives.展开更多
In two-dimensional van der Waals materials,electronic band structures are highly sensitive to both twist angle and structural reconstruction[[1],[2],[3],[4],[5],[6]].The exceptional control of the interlayer twist ang...In two-dimensional van der Waals materials,electronic band structures are highly sensitive to both twist angle and structural reconstruction[[1],[2],[3],[4],[5],[6]].The exceptional control of the interlayer twist angle in two-dimensional van der Waals materials leads to the discovery of different emergent phenomena.Therefore,the effects of the twist angle on the electronic properties have been studied extensively[1,2].展开更多
Graphdiyne(GDY),a rising star of carbon allotrope with sp-/sp?.hybridized one-atom-thick all-carbon two-dimensional(2D)network,has shown numerous unique structure and fascinating properties.Since the first successful ...Graphdiyne(GDY),a rising star of carbon allotrope with sp-/sp?.hybridized one-atom-thick all-carbon two-dimensional(2D)network,has shown numerous unique structure and fascinating properties.Since the first successful synthesis of GDY in 2010,GDY research has made a series of great progresses,and promoted the fundamental researches and practical applications in various fields of chemistry,physics,information science,material science,life science and environmental science and so on.展开更多
基金supported bythe Science and Technology Commission of Shanghai Municipality (Grant No.24CL2901702)The numerical calculations were performed at the Supercomputer Center (Project No.2024-Cb-0042)Institute for Solid State Physics,the University of Tokyo。
文摘Heat dissipation and thermal switches are vital for adaptive cooling and extending the lifespan of electronic devices and batteries. In this work, we conducted high-throughput investigations on the thermal transport of 24 experimentally realized two-dimensional(2D) materials and their potential as thermal switches, leveraging machine-learning-assisted strain engineering and phonon transport simulations. We identified several highperformance thermal switches with ratios exceeding 2, with germanene(Ge) achieving an ultrahigh ratio of up to9.64 within the reversible deformation range. The underlying mechanism is strain-induced bond softening, which sensitively affects anharmonicity represented by three-and four-phonon scattering. The widespread occurrence of four-phonon scattering was confirmed in the thermal transport of 2D materials. Opposite switching trends were discovered, with 2D transition metal dichalcogenide materials showing negative responses to tensile strain while buckled 2D elemental materials showed positive responses. We further proposed a screening descriptor based on strain-induced changes in the Gr¨uneisen parameter for efficiently identifying new high-performance thermal switch materials. This work establishes a paradigm for thermal energy control in 2D materials through strain engineering, which may be experimentally realized in the future via bending, substrate mismatch, and related approaches, thereby laying a robust foundation for further developments and applications.
基金supported by the High-level Talent Research Start-up Project Funding of Henan Academy of Sciences(Project No.241827012)the National Natural Science Foundation of China(Grant Nos.U22A6005 and 62271450)+1 种基金the National Key Research and Development Program of China(Grant Nos.2021YFA1301502,2024YFA1408701,and 2024YFA1408403)the Synergetic Extreme Condition User Facility(SECUF,https://cstr.cn/31123.02.SECUF)。
文摘The precise control of wrinkles and strain gradients in nanofilm is of significant interest due to their profound influence on electronic band structures and spin states.Here,we employ ultrafast electron diffraction(UED)to study the picosecond-scale dynamics of laser-induced bending in 2H-MoTe2 thin films.
基金support from the National Natural Science Foundation of China(Grants 22125903,22439003,22209173,22309176 and 22409196)the National Key R&D Program of China(Grant 2023YFB4005204)+6 种基金the Science and Technology Major Project of Liaoning Province(Grant No.2024JH1/11700012)the Energy Revolution S&T Program of Yulin Innovation Institute of Clean Energy(Grant E411050316)Liaoning Binhai Laboratory(Grant No.LBLD-2024-04)DICP(DICP I202471,DICP I202460)the State Key Laboratory of Catalysis(No.2024SKL-A-001)China National Postdoctoral Program for Innovative Talents(BX20240361)the Natural Science Foundation of Liaoning Province(2023BS006 and 2024-BSBA-31).
文摘CONSPECTUS:Two-dimensional(2D)materials form a large and diverse family of materials with extremely rich compositions,ranging from graphene to complex transition metal derivatives.They exhibit unique physical,chemical,and electronic properties,making 2D materials highly promising in the fields of sustainable energy storage and electrocatalysis.Although significant progress has been made in the design and performance optimization of 2D materials,challenges persist,particularly in energy storage and electrocatalysis.A key issue is the restacking or aggregation of these materials in the powder form,which hinders ion transport and reduces their overall performance by limiting the effective surface area.
基金funding by the German Research Foundation(DFG)through the NFDI consortium FAIRmat,project 460197019.
文摘With the rapidly increasing amount of materials data being generated in a variety of projects,efficient and accurate classification of atomistic structures is essential.A current barrier to effective database queries lies in the often ambiguous,inconsistent,or completely missing classification of existing data,highlighting the need for standardized,automated,and verifiable classification methods.This work proposes a robust solution for identifying and classifying a wide spectrum of materials through an iterative technique,called symmetry-based clustering(SBC).Because SBC is not a machine learningbased method,it requires no prior training.Instead,it identifies clusters in atomistic systems by automatically recognizing common unit cells.We demonstrate the potential of SBC to provide automated,reliable classification and to reveal well-known symmetry properties of various materials.Even noisy systems are shown to be classifiable,showing the suitability of our algorithm for real-world data applications.The software implementation is provided in the open-source Python package,MatID,exploiting synergies with popular atomic-structure manipulation libraries and extending the accessibility of those libraries through the NOMAD platform.
基金supported by the Iran National Science Foundation(INSF)under Project No.4044100the Collaborative Research Center CRC/TRR 227 of the Deutsche Forschungsgemeinschaft(DFG),and the European Union(EFRE)via Grant No.ZS/2016/06/79307.
文摘Understanding the interplay between screening,electronic correlations,and collective excitations is essential for the design of two-dimensional quantum materials.Here,we present a comprehensive first-principles study of more than 60 MA_(2)Z_(4)monolayers,encompassing semiconducting,metallic,cold-metallic,magnetic,and topological phases.Using the constrained random phase approximation(cRPA),wecompute material-specific effectiveCoulomb interaction parametersU,U0,and J,including their spatial dependence across distinct correlated subspaces defined by local coordination and crystal symmetry.In semiconducting compounds,long-range nonlocal interactions persist,revealing unconventional screening and suggesting strong excitonic effects beyond simple dielectricmodels.In cold-metallic systems,sizable long-range Coulomb interactions remain despite the presence of free carriers,highlighting their atypical metallic screening.Among 33-valence-electron compounds,we find U^(eff)>W in theβ2 phase,indicating proximity to charge-density-wave or Mott instabilities.Several V-and Nb-based systems exhibit intermediate-to-strong correlation strength,with U/W>1 in multiple cases.Using cRPA-derived Stoner parameters,we identify magnetic instabilities in various V-,Nb-,Cr-,andMn-based compounds.Finally,selected cold-metallic systems display plasmon dispersions that deviate from the conventional√q behavior,revealing nearly non-dispersive low-energy modes.These results position MA_(2)Z_(4)monolayers as a versatile platform for investigating correlation-driven instabilities and emergent collective behavior in two dimensions.
基金RSF No.24-73-10055 for financial support of the development of ML interatomic potential for Mo-S system and calculation of dynamical properties of newly found materialsA.V.A.is supported by the Ministry of Science and Higher Education(FSMG-2025-0005)+3 种基金D.G.K.acknowledges financial support from the federal budget of the Russian Ministry of Science and Higher Education(No.125020401357-4)A.R.O.gratefully acknowledges support from Russian Science Foundation(grant 24-43-00162)K.S.N acknowledges support from the Ministry of Education,Singapore under Research Centre of Excellence award to the Institute for Functional Intelligent Materials,I-FIM(project No.EDUNC-33-18-279-V12)and under the Tier 3 program(MOE-MOET32024-0001)the National Research Foundation,Singapore under its AI Singapore Programme(AISG Award No:AISG3-RP-2022-028).
文摘Two-dimensional(2D)materials attract considerable attention due to their remarkable electronic,mechanical and optical properties.Despite their use in combination with substrates in practical applications,computational studies often neglect the effects of substrate interactions for simplicity.This study presents a novel method for predicting the atomic structure of 2D materials on substrates by combining an evolutionary algorithm,a lattice-matching technique,an automated machinelearning interatomic potentials training protocol,and the ab initio thermodynamics approach.Using the molybdenum-sulfur system on a sapphire substrate as a case study,we reveal several new stable and metastable structures,including previously known 1H-MoS_(2)and newly found Pmma Mo_(3)S_(2),P1^(-)Mo_(2)S,P2_(1)m Mo_(5)S_(3),and P_(4)mm Mo_(4)S,where the Mo_(4)S structure is specifically stabilized by interaction with the substrate.Finally,we use the ab initio thermodynamics approach to predict the synthesis conditions of the discovered structures in the parameter space of the commonly used chemical vapor deposition technique.
基金supported by the National Key Basic Research and Development Program of China,China(No.2024YFA1409100)support by the National Natural Science Foundation of China,China(Nos.52473302 and 12461160252)+4 种基金Guangdong Innovative and Entrepreneurial Research Team Program,China(No.2019ZT08C044)Guangdong Basic Science Foundation,China(2023B1515120039)Shenzhen Science and Technology Program,China(No.20200925161102001)the Science,Technology and Innovation Commission of Shenzhen Municipality,China(No.ZDSYS20190902092905285)Quantum Science Strategic Special Project from the Quantum Science Center of Guangdong-Hong Kong-Macao Greater Bay Area,China(No.GDZX2301006).
文摘Transmission electron microscopy(TEM)is an indispensable tool for elucidating the intrinsic atomic structures of materials and provides deep insights into defect dynamics,phase transitions,and nanoscale structural details.While numerous intriguing physical properties have been revealed in recently discovered two-dimensional(2D)quantummaterials,many exhibit significant sensitivity towater and oxygen under ambient conditions.This inherent instability complicates sample preparation for TEM analysis and hinders accurate property measurements.This review highlights recent technical advancements to preserve the intrinsic structures of water-and oxygen-sensitive 2D materials for atomic-scale characterizations.A critical development discussed in this review is implementing an inert gas-protected glovebox integrated system(GIS)designed specifically for TEM experiments.In addition,this review emphasizes air-sensitivematerials such as 2D transitionmetal dichalcogenides,transition metal dihalides and trihalides,and low-dimensional magnetic materials,demonstrating breakthroughs in overcoming their environmental sensitivity.Furthermore,the progress in TEM characterization enabled by the GIS is analyzed to provide a comprehensive overview of state-of-the-art methodologies in this rapidly advancing field.
基金supported by the Federal Ministry of Education and Research of Germany in the framework of the Palestinian-German Science Bridge (BMBF grant number 01DH16027)support by the Deutsche Forschungsgemeinschaft (DFG, German Research Foundation)—TRR 288—422213477 (projects B06 and A12), TRR 173/2—268565370 (projects A11 and A01), CRC 1238 - 277146847 (Project C01)+1 种基金the Sino-German research project DISTOMAT (MO 1731/10-1)This work was supported by the EIC Pathfinder OPEN grant 101129641 “OBELIX” and the king Abdullah university of science and technology (KAUST) under award 2024-CRG12-6480. We also gratefully acknowledge the Jülich Supercomputing Centre and RWTH Aachen University for providing computational resources under projects jiff40 and jara0062.
文摘The design of spin-orbit torque properties in two-dimensional(2D)materials presents one of the challenges of modern spintronics.In this context,2D layers involving rare-earth ions−which give rise to robust magnetism,exhibit pronounced orbital polarization of the states,and carry strong spin-orbit interaction—hold particular promise.Here,we investigate ferromagnetic Janus H-phase monolayers of 4f-Eu rare-earth dichalcogenides EuSP,EuSSe,and EuSCl using first-principles calculations.We demonstrate that all compounds exhibit significant spin-orbit torques which originate predominantly in the colossal current-induced orbital response on the Eu f-electrons.Moreover,we demonstrate that the corresponding orbital torques can be used to drive strong in-plane currents of orbital angular momentum with non-trivial direction of orbital polarization,constituting the effect of in-plane orbital pumping.We provide an interpretation of this effect in terms of orbital-to-orbital-curent conversion,and draw a simple qualitative picture of orbital pumping by magnetization dynamics in two dimensional systems.Our findings promote f-orbital-based 2D materials as a promising platform for in-plane orbital pumping and spin-orbit torque applications,and motivate further research on educated design of orbital properties for orbitronics with 2D materials.
基金financial support from National Key Research and Development Program of China(Nos.2023YFB3611400,2024YFB2808200)National Natural Science Foundation of China(62450123,62375042,62475230)Sichuan Science and Technology Program(No.2024NSFSC1445).
文摘With the rapid advancement of the information age,the demand for multi-dimensional light information detection has significantly increased.Traditional Fourier-transform infrared(FTIR)spectrometers and pooptical power,andlarimeters,due to their bulky structure,are no longer suitable for emerging fields such as medical diagnostics,secure communications,and autonomous driving.As a result,there is a pressing need to develop new miniaturized on-chip devices.The abundant two-dimensional(2D)materials,with their unique light-matter interactions,offer the potential to construct high-dimensional spatial mappings of incident light,paving the way for the development of novel ultra-compact multi-dimensional deep optical sensing technologies.Here,we review the interconnections of multi-dimensional information and their relationship with 2D materials.We then focus on recent advances in the development of novel dimensional detectors based on 2D materials,covering dimensions such as intensity,time,space,polarization,phase angle,and wavelength.Furthermore,we discuss cutting-edge technologies in multi-dimensional fusion detection and highlight future technological prospects,with a particular emphasis on on-chip integration and future development.
文摘Two-dimensional(2D)transition metal dichalcogenides(TMDs),which allow atomic-scale manipulation,have supe-rior electrical and optical properties that challenge the limits of traditional bulk semiconductors like silicon^([1,2]).As a repre-sentative TMD and a promising 2D channel material for high-performance,scalable p-type transistors,tungsten diselenide(WSe_(2))has attracted considerable academic and industrial interest for its potential in advanced complementary metal−oxide−semiconductor(CMOS)logic technology and in extending Moore’s Law^([3−7]).
基金supported by the National Research Foundation of Korea(NRF)grants(RS-2023-00283500,RS-2025-00559639,RS-2024-00412690,RS-2023-00254055)the Samsung Science and Technology Foundation(SSTP-BA2102-05)+6 种基金the MSIT(Ministry of Science and ICT)under the ITRC(Information Technology Research Center)support program(IITP-2022-RS-2022-00164799)J.R.acknowledges the POSCO-POSTECH-RIST Convergence Research Center program funded by POSCO,and the National Research Foundation(NRF)grant(RS-2024-00356928)funded by the Ministry of Science and ICT(MSIT)of the Korean government.D.K.O.acknowledges the Hyundai Motor Chung Mong-Koo fellowshipJ.M.acknowledges the Presidential Sejong fellowship(RS-2023-00252778)funded by the MSIT of the Korean governmentY.Kim acknowledges the Hyundai Motor Chung Mong-Koo fellowship and the NRF PhD fellowship(NRF-2022R1A6A3A13066251)funded by the Ministry of Education(MOE)of the Korean government.T.K.and J.K.acknowledge the support from the Institute of Basic Science(IBS-R034-D1)J.K.acknowledges the support from the National Research Foundation of Korea grants(NRF-2023R1A2C2007998)supported by the MSIT(Ministry of Science and ICT),Korea,under the ITRC(Information Technology Research Center)support program(IITP-2023-RS-2022-00164799)supervised by the IITP(Institute for Information&Communications Technology Planning&EvaluationM.T.,A.N.A.,and V.K.acknowledge support from the Priority 2030 Federal Academic Leadership Program(angle-resolved measurements)and the Russian Science Foundation,project 22-72-10047(sample fabrication).
文摘Dramatic fluorescence enhancement in two-dimensional(2D)van der Waals materials(vdWMs)coupled to plasmonic nanostructures has the potential to enable ultrathin,flexible,and high-brightness illumination devices.However,addressing the limitation of locally scattered small plasmon-enhanced areas remains challenging.Here,we present a 2D plasmonic enhancement of photoluminescence(PL)spanning nearly 800μm^(2),enabled by surface lattice resonance(SLR)in a 2D vdWM-Au slot lattice hybrid.The Au slot lattice is designed and fabricated using Babinet’s principle and Rayleigh’s anomaly to maximize radiative decay rate and induce non-local photo-excitation in a MoSe_(2)monolayer.For emitted PL coupled with SLR,enhanced by up to 32-fold,we investigate its in-plane directivity and long-range propagation using angle-and space-resolved spectroscopic PL measurements.Our experiment reveals that a nearly 800μm^(2)2D luminescent sheet can be achieved regardless of the size of the MoSe_(2)crystal,even with a sub-μm^(2)flake.This work provides a new type of ultrabright,large-area 2D luminescent material,suitable for a range of optical illumination,communication,and sensing devices.
基金supported by the National Natural Science Foundation of China(No.11304184)the Shandong University of Technology and Zibo City Integration Development Project(No.2019ZBXC120)。
文摘Based on the nonlinear saturable absorption properties(NSAPs)of a two-dimensional(2D)material of antimony selenide(Sb_(2)Se_(3)),a Q-switched erbium-doped fiber(EDF)laser is systematically demonstrated.The Sb_(2)Se_(3)nano sheets are prepared by liquid-phase exfoliation(LPE)method.After the sandwich-structured Sb_(2)Se_(3)saturable absorber(SA)is fabricated,the NSAPs are characterized and the modulation depth,the saturation intensity and the unsaturated loss are determined to be 25.2%,2.02 MW/cm^(2),and 3.29%,respectively.When the as-prepared Sb_(2)Se_(3)-SA is integrated into the ring cavity,the laser operates at a stable Q-switching regime in the pump power range of 100—400 mW.The laser oscillates at the central wavelength of 1558.48 nm with a 3 dB bandwidth of 2.32 nm.Take the advantages of the Sb_(2)Se_(3)-SA,the pulse duration can be compressed from 40.49 kHz to 128.12 kHz.At the pump power of 400 mW,the Q-switching laser gives the narrowest pulse duration the highest average output power,the largest pulse energy,and the signal-to-noise ratio(SNR)of 0.93μs,2.16 mW,16.89 nJ,and 53 dB,respectively.Our new attempt on Sb_(2)Se_(3)-based Q-switched EDF laser,combining the existing mode-locking achievements,proves that Sb_(2)Se_(3)is a powerful candidate for pulse compression due to the characteristics of high modulation depth and high stability.
基金the support from an Empa interal research grant.
文摘Rechargeable lithium-sulfur(Li-S)batteries have attracted significant research attention due to their high capacity and energy density.However,their commercial applications are still hindered by challenges such as the shuttle effect of soluble lithium sulfide species,the insulating nature of sulfur,and the fast capacity decay of the electrodes.Various efforts are devoted to address these problems through questing more conductive hosts with abundant polysulfide chemisorption sites,as well as modifying the separators to physically/chemically retard the polysulfides migration.Two dimensional transition metal carbides,carbonitrides and nitrides,so-called MXenes,are ideal for confining the polysulfides shuttling effects due to their high conductivity,layered structure as well as rich surface terminations.As such,MXenes have thus been widely studied in Li-S batteries,focusing on the conductive sulfur hosts,polysulfides interfaces,and separators.Therefore,in this review,we summarize the significant progresses regarding the design of multifunctional MXene-based Li-S batteries and discuss the solutions for improving electrochemical performances in detail.In addition,challenges and perspectives of MXenes for Li-S batteries are also outlined.
基金supported by the National Natural Science Foundation of China(No.61575059,No.61675062,No.21501038)the Fundamental Research Funds for the Central Universities(No.JZ2018HGPB0275,No.JZ2018HGTA0220,and No.JZ2018HGXC0001).
文摘In this study,we have developed a high-sensitivity,near-infrared photodetector based on PdSe2/GaAs heterojunction,which was made by transferring a multilayered PdSe2 film onto a planar GaAs.The as-fabricated PdSe2/GaAs heterojunction device exhibited obvious photovoltaic behavior to 808 nm illumination,indicating that the near-infrared photodetector can be used as a self-driven device without external power supply.Further device analysis showed that the hybrid heterojunction exhibited a high on/off ratio of 1.16×10^5 measured at 808 nm under zero bias voltage.The responsivity and specific detectivity of photodetector were estimated to be 171.34 mA/W and 2.36×10^11 Jones,respectively.Moreover,the device showed excellent stability and reliable repeatability.After 2 months,the photoelectric characteristics of the near-infrared photodetector hardly degrade in air,attributable to the good stability of the PdSe2.Finally,the PdSe2/GaAs-based heterojunction device can also function as a near-infrared light sensor.
基金supported by National University of Singapore No. CENGas R-261-508-001-646)Ministry of Education – Singapore ( 13No. MOE Ac RF Tier 1 R-279-000-472-112)
文摘Two-dimensional（2 D） materials have attracted increasing attentions recently due to their unique physical and chemical properties. We herein report the synthesis of four chemically stable 2 D covalent organic nanosheets（CONs） with large lateral sizes（up to 200 mm） and high aspect ratios（〉20 000） at the air-water interface through the Langmuir-Blodgett method. These CONs exhibit good crystallinity proved by high resolution transmission electron microscopy（HRTEM） and selected area electron diffraction（SAED）. In addition, the hydrophobicity of these CONs can be systematically adjusted by the introduction of various functional groups, making them suitable as functional coating and membrane materials.
基金the National Natural Science Foundation of China(Nos.21872169,91845109,21688102,and 21825203)the National Key R&D Program of China(No.2016YFA0200200)+2 种基金Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB17020000)China Postdoctoral Science Foundation(No.2019M651997)Natural Science Foundation of Jiangsu Province(No.BK20200257).
文摘The synthesis of high-quality ultrathin overlayers is critically dependent on the surface structure of substrates,especially involving the overlayer–substrate interaction.By using in situ surface measurements,we demonstrate that the overlayer–substrate interaction can be tuned by doping near-surface Ar nanobubbles.The interfacial coupling strength significantly decreases with near-surface Ar nanobubbles,accompanying by an“anisotropic to isotropic”growth transformation.On the substrate containing near-surface Ar,the growth front crosses entire surface atomic steps in both uphill and downhill directions with no difference,and thus,the morphology of the two-dimensional(2D)overlayer exhibits a round-shape.Especially,the round-shaped 2D overlayers coalesce seamlessly with a growth acceleration in the approaching direction,which is barely observed in the synthesis of 2D materials.This can be attributed to the immigration lifetime and diffusion rate of growth species,which depends on the overlayer–substrate interaction and the surface catalysis.Furthermore,the“round to hexagon”morphological transition is achieved by etching-regrowth,revealing the inherent growth kinetics under quasi-freestanding conditions.These findings provide a novel promising way to modulate the growth,coalescence,and etching dynamics of 2D materials on solid surfaces by adjusting the strength of overlayer–substrate interaction,which contributes to optimization of large-scale production of 2D material crystals.
基金the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation programme Grant No.773122(LIMA)and Grant agreement No.951786(NOMAD CoE)A high-performance computing infrastructure for data-driven research on sustainable energy materials,Grant no.NNF22OC0078009.K.S.T.is a Villum Investigator supported by VILLUM FONDEN(grant no.37789).
文摘We conduct a systematic investigation of the role of Hubbard U corrections in electronic structure calculations of two-dimensional(2D)materials containing 3d transition metals.Specifically,we use density functional theory(DFT)with the PBE and PBE+U approximations to calculate the crystal structure,band gaps,and magnetic parameters of 638 monolayers.Based on a comprehensive comparison to experiments we first establish that the inclusion of the U correction worsens the accuracy for the lattice constants.Consequently,PBE structures are used for subsequent property evaluations.The band gaps show a significant dependence on U.In particular,for 134(21%)of the materials the U parameter induces a metal-to-insulator transition.For the magnetic materials we calculate the magnetic moment,magnetic exchange coupling,and magnetic anisotropy parameters.In contrast to the band gaps,the size of the magnetic moments shows only weak dependence on U.Both the exchange energies and magnetic anisotropy parameters are systematically reduced by theU correction.On this basis we conclude that the Hubbard U correction will lead to lower predicted Curie temperatures in 2D materials.All the calculated properties are available in the Computational 2D Materials Database(C2DB).
基金The project was supported by Equipment Pre-research Key Laboratory Fund(No.6142020305)The authors would like to thank Shiyanjia Lab(www.shiyanjia.com)for the support of XPS test.
文摘Hexagonal boron nitride nanosheets(HBNNSs)have huge potential in the field of coating materials owing to their remarkable chemical stability,mechanical strength and thermal conductivity.Thin-layer hBNNSs were obtained by a liquid-phase exfoliation of h-BN powders and incorporated into EVA coatings for improving the safety performance of 1,3,5,7-tetranitro-1,3,5,7-tetrazocane(HMX).HBNNSs and ethylene-vinyl acetate copolymer(EVA)were introduced to HMX by a solvent-slurry process.For comparison,the HMX/EVA and HMX/EVA/graphene(HMX/EVA/G)composites were also prepared by a similar process.The morphology,crystal form,surface element distribution,thermal decomposition property and impact sensitivity of HMX/EVA/hBNNSs composites were contrastively investigated.Results showed that as prepared HMX/EVA/hBNNSs composites were well coated with hBNNSs and EVA,and exhibited better thermal stability and lower impact sensitivity than that of HMX/EVA and HMX/EVA/G composites,suggesting superior performance of desensitization of hBNNSs in explosives.
基金supported by the National Natural Science Foundation of China(12425405,12404198,12141401,and 12174291)the National Key R&D Program of China(2021YFA1400100 and 2021YFA1401900)+4 种基金the Major Program(JD)of Hubei Province(2023BAA020)the Knowledge Innovation Program of Wuhan Science and Technology Bureau(2022013301015171)“the Fundamental Research Funds for the Central Universities”(310400209521)the China National Postdoctoral Program for Innovative Talents(BX20240040)the China Postdoctoral Science Foundation(2023M740296).
文摘In two-dimensional van der Waals materials,electronic band structures are highly sensitive to both twist angle and structural reconstruction[[1],[2],[3],[4],[5],[6]].The exceptional control of the interlayer twist angle in two-dimensional van der Waals materials leads to the discovery of different emergent phenomena.Therefore,the effects of the twist angle on the electronic properties have been studied extensively[1,2].
文摘Graphdiyne(GDY),a rising star of carbon allotrope with sp-/sp?.hybridized one-atom-thick all-carbon two-dimensional(2D)network,has shown numerous unique structure and fascinating properties.Since the first successful synthesis of GDY in 2010,GDY research has made a series of great progresses,and promoted the fundamental researches and practical applications in various fields of chemistry,physics,information science,material science,life science and environmental science and so on.
