We describe in this paper the fabrication of two- and one-dimensional nanostructures with organic molecular beam epitaxy （OMBE） principle based on controlled selfassembly by using adsorbate-substrate and intennolecu...We describe in this paper the fabrication of two- and one-dimensional nanostructures with organic molecular beam epitaxy （OMBE） principle based on controlled selfassembly by using adsorbate-substrate and intennolecular interactions that are important in molecular fabrication. Cu（100） single crystal was used as substrate in fabricating molecular nanostructures. Scanning tunneling microscopy （STM） experiments confirmed that Zn-tetra- [3,5-di-t-butylphenyl]porphyrin-molecules can be used to fabricate both monolayer and molecular wire on Cu（100） surface simultaneously, and the latter is arranged on the terrace edges. We herein briefly discuss the selectivity in terms of a mechanism in which the highest occupied and lowest unoccupied molecular orbitals （HOMO and LUMO） of the molecules interact with the surface.展开更多
We investigate the electronic-transport properties of two-dimensional monolayer films from Au-P-Au molecular junction to Au-Si-Au molecular junction using elastic scattering Green＇s function theory. In the process of...We investigate the electronic-transport properties of two-dimensional monolayer films from Au-P-Au molecular junction to Au-Si-Au molecular junction using elastic scattering Green＇s function theory. In the process of replacing the P atoms with Si atoms every other line from the middle of monolayer blue phosphorus molecular structure, the substitution of Si atoms changes the properties of Au-P-Au molecular junction significantly. Interestingly, the current value has a symmetric change as a parabolic curve with the peak appearing in Au-Si_1P_1-Au molecular junction, which provides the most stable current of 15.00 nA in a wide voltage range of 0.70-2.70 V.Moreover, the current-voltage characteristics of the structures indicate that the steps tend to disappear revealing the property similar to metal when the Si atoms dominate the molecular junction.展开更多
Directly correlating the morphology and composition of interfacial water is vital not only for studying water icing under critical conditions but also for understanding the role of protein–water interac-tions in bio-...Directly correlating the morphology and composition of interfacial water is vital not only for studying water icing under critical conditions but also for understanding the role of protein–water interac-tions in bio-relevant systems.In this study,we present a model system to study two-dimensional(2D)water layers under ambient conditions by using self-assembled monolayers(SAMs)supporting the physisorp-tion of the Cytochrome C(Cyt C)protein layer.We observed that the 2D island-like water layers were uniformly distributed on the SAMs as characterized by atomic force microscopy,and their composition was confirmed by nano-atomic force microscopy-infrared spectroscopy and Raman spectroscopy.In addition,these 2D flakes could grow under high-humidity conditions or melt upon the introduction of a heat source.The formation of these flakes is attributed to the activation energy for water desorption from the Cyt C being nearly twofold high than that from the SAMs.Our results provide a new and effective method for further understanding the water–protein interactions.展开更多
We report the discovery of bistable polar states with switchable polarization in the Janus monolayer 1T-MoSSe,induced by symmetry breaking in its chalcogen atomic layers.Our results demonstrate that Janus 1T-MoSSe exh...We report the discovery of bistable polar states with switchable polarization in the Janus monolayer 1T-MoSSe,induced by symmetry breaking in its chalcogen atomic layers.Our results demonstrate that Janus 1T-MoSSe exhibits two out-of-plane bistable polar states with switchable polarization,rather than polarization emerging from a non-polar phase,which represents an unconventional form of ferroelectric-like behavior.First-principles calculations and phenomenological modeling reveal that the inequivalent stacking of sulfur and selenium(S/Se)atoms breaks central inversion symmetry,activating non-degenerate phonon modes at the K-point(K_(2)/K_(3))that drive the structural transformation between metastable d1TS and d1TSe phases.This coupling enables bipolar control of out-of-plane polarization through atomic displacements and charge redistribution,resulting in a polarization change ofΔP≈±0.3μC/cm^(2).The Landau free energy analysis indicates that anharmonic terms and inter-mode coupling generate an asymmetric double-well potential,which is essential for the stabilization of bistable polar states.Molecular dynamics simulations show that the d1TS phase remains stable at high temperatures,whereas the d1TSe phase undergoes an irreversible phase transition near 300 K,accompanied by a Peierls-like distortion of the Mo atomic chain.This transition is driven by differences in electronegativity,atomic radius,and d-p orbital hybridization between S and Se.Our findings establish a theoretical framework for engineering nonlinear responses in two-dimensional(2D)ferroelectrics and suggest that low-energy polarization reversal at room temperature can be achieved through strain or electric-field control,offering promising opportunities for non-volatile memory and piezoelectric sensing applications.展开更多
Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)...Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)and CO_(2) electroreduction(CO_(2)ER)to valuable chemicals.Under such context,this work reported computational efforts to design promising electrocatalyst for HER and CO_(2)ER based on the swarm-intelligence algorithm.Among the family of transition-metal phosphides(TMPs),Pt_(2)P_(3) monolayer has been identified as excellent bifunctional catalysts due to high stability,excellent conductivity and superior catalytic performance.Different from typical d-block catalysts,p-band center presented by P atoms within Pt_(2)P_(3) monolayer plays the essential role for its reactivity towards HER and CO_(2)ER,underlining the key value of p-electrons in advanced catalyst design and thus providing a promising strategy to further develop novel catalysts made of p-block elements for various energy applications.展开更多
Two-dimensional （2D） ferromagnetic （FM） materials have great potential for applications in next-generation spin- tronic devices. Since most 2D FM materials come from van der Waals crystals, stabilizing them on a c...Two-dimensional （2D） ferromagnetic （FM） materials have great potential for applications in next-generation spin- tronic devices. Since most 2D FM materials come from van der Waals crystals, stabilizing them on a certain substrate without killing the ferromagnetism is still a challenge. Through systematic first-principles calculations, we proposed a new family of 2D FM materials which combines TaX （X= S, Se or Te） monolayer and A1203（0001） substrate. The TaX monolayers provide magnetic states and the A1203（0001） substrate stabilizes the former. Interestingly, the A1203（0001） substrate leads to a metal-to-insulator transition in the TaX monolayers and induces a band gap up to 303 meV. Our study paves the way to explore promising 2D FM materials for practical applications in spintronics devices.展开更多
As emerging two-dimensional(2D)materials,carbides and nitrides(MXenes)could be solid solutions or organized structures made up of multi-atomic layers.With remarkable and adjustable electrical,optical,mechanical,and el...As emerging two-dimensional(2D)materials,carbides and nitrides(MXenes)could be solid solutions or organized structures made up of multi-atomic layers.With remarkable and adjustable electrical,optical,mechanical,and electrochemical characteristics,MXenes have shown great potential in brain-inspired neuromorphic computing electronics,including neuromorphic gas sensors,pressure sensors and photodetectors.This paper provides a forward-looking review of the research progress regarding MXenes in the neuromorphic sensing domain and discussed the critical challenges that need to be resolved.Key bottlenecks such as insufficient long-term stability under environmental exposure,high costs,scalability limitations in large-scale production,and mechanical mismatch in wearable integration hinder their practical deployment.Furthermore,unresolved issues like interfacial compatibility in heterostructures and energy inefficiency in neu-romorphic signal conversion demand urgent attention.The review offers insights into future research directions enhance the fundamental understanding of MXene properties and promote further integration into neuromorphic computing applications through the convergence with various emerging technologies.展开更多
Compared to the well-studied two-dimensional(2D)ferroelectricity,the appearance of 2D antiferroelectricity is much rarer,where local dipoles from the nonequivalent sublattices within 2D monolayers are oppositely orien...Compared to the well-studied two-dimensional(2D)ferroelectricity,the appearance of 2D antiferroelectricity is much rarer,where local dipoles from the nonequivalent sublattices within 2D monolayers are oppositely oriented.Using NbOCl_(2) monolayer with competing ferroelectric(FE)and antiferroelectric(AFE)phases as a 2D material platform,we demonstrate the emergence of intrinsic antiferroelectricity in NbOCl_(2) monolayer under experimentally accessible shear strain,along with new functionality associated with electric field-induced AFE-to-FE phase transition.Specifically,the complex configuration space accommodating FE and AFE phases,polarization switching kinetics,and finite temperature thermodynamic properties of 2D NbOCl_(2) are all accurately predicted by large-scale molecular dynamics simulations based on deep learning interatomic potential model.Moreover,room temperature stable antiferroelectricity with low polarization switching barrier and one-dimensional collinear polarization arrangement is predicted in shear-deformed NbOCl_(2) monolayer.The transition from AFE to FE phase in 2D NbOCl_(2) can be triggered by a low critical electric field,leading to a double polarization–electric(P–E)loop with small hysteresis.A new type of optoelectronic device composed of AFE-NbOCl_(2) is proposed,enabling electric“writing”and nonlinear optical“reading”logical operation with fast operation speed and low power consumption.展开更多
Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-...Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-mediated e–h recombination the dominant decay pathway.In this work,nonradiative e–h recombination within excitons in monolayer MoS2 is investigated using first-principles simulations that combine nonadiabatic molecular dynamics with𝐺𝑊and real-time Bethe–Salpeter equation(BSE)propagation.A two-step process is identified:rapid intervalley redistribution induced by exchange interaction,followed by slower phonon-assisted recombination facilitated by exciton binding.By selectively removing the screened Coulomb and exchange terms from the BSE Hamiltonian,their respective contributions are disentangled—exchange interaction is found to increase the number of accessible recombination pathways,while binding reduces the excitation energy and enhances nonradiative decay.A reduction in recombination lifetime by over an order of magnitude is observed due to the excitonic many-body effects.These findings provide microscopic insights for understanding and tuning exciton lifetimes in 2D transition-metal dichalcogenides.展开更多
The fundamental momentum conservation requirement q - 0 for the Raman process is relaxed in the nanocrystal- lites （NCs）, and phonons away from the Brillouin-zone center will be involved in the Raman scattering, whi...The fundamental momentum conservation requirement q - 0 for the Raman process is relaxed in the nanocrystal- lites （NCs）, and phonons away from the Brillouin-zone center will be involved in the Raman scattering, which is well-known as the phonon confinement effect in NCs. This usually gives a downshift and asymmetric broadening of the Raman peak in various NCs. Recently, the A1 mode of 1L MoS2 NCs is found to exhibit a blue shift and asymmetric broadening toward the high-frequency side [Chem. Soc. Rev. 44 （2015） 2757 and Phys. Rev. B 91 （2015） 195411]. In this work, we carefully check this issue by studying Raman spectra of lL MoS2 NCs prepared by the ion implantation technique in a wide range of ion-implanted dosage. The same confinement coefficient is used for both E＇ and A＇1 modes in 1L MoS2 NCs since the phonon uncertainty in an NC is mainly determined by its domain size. The asymmetrical broadening near the A＇1 and E＇ modes is attributed to the appearance of defect-activated phonons at the zone edge and the intrinsic asymmetrical broadening of the two modes, where the anisotropy of phonon dispersion curves along Г-K and Г- M is also considered. The photoluminescence spectra confirm the formation of small domain size of 1L MoS2 nanocrystallites in the ion-implanted 1L MoS2. This study provides not only an approach to quickly probe phonon dispersion trends of 2D materials away from Г by the Raman scattering of the corresponding NCs, but also a reference to completely understand the confinement effect of different modes in various nanomaterials.展开更多
We report on the formation of two-dimensional monolayer AgTe crystal on Ag(111)substrates.The samples are prepared in ultrahigh vacuum by deposition of Te on Ag(111)followed by annealing.Using a scanning tunneling mic...We report on the formation of two-dimensional monolayer AgTe crystal on Ag(111)substrates.The samples are prepared in ultrahigh vacuum by deposition of Te on Ag(111)followed by annealing.Using a scanning tunneling microscope(STM)and low electron energy diffraction(LEED),we investigate the atomic structure of the samples.The STM images and the LEED pattern show that monolayer AgTe crystal is formed on Ag(111).Four kinds of atomic structures of AgTe and Ag(111)are observed:(i)flat honeycomb structure,(ii)bulked honeycomb,(iii)stripe structure,(iv)hexagonal structure.The structural analysis indicates that the formation of the different atomic structures is due to the lattice mismatch and relief of the intrinsic strain in the AgTe layer.Our results provide a simple and convenient method to produce monolayer AgTe atomic crystal on Ag(111)and a template for study of novel physical properties and for future quantum devices.展开更多
Two-dimensional multiferroics,which simultaneously possess ferroelectricity and magnetism in a single phase,are well-known to possess great potential applications in nanoscale memories and spintronics.On the basis of ...Two-dimensional multiferroics,which simultaneously possess ferroelectricity and magnetism in a single phase,are well-known to possess great potential applications in nanoscale memories and spintronics.On the basis of first-principles calculations,a CrNCl_(2) monolayer is reported as an intrinsic multiferroic.The CrNCl_(2) has an antiferromagnetic ground state,with a N´eel temperature of about 88 K,and it exhibits an in-plane spontaneous polarization of 200 pC/m.The magnetic moments of CrNCl_(2) mainly come from the dxy orbital of the Cr cation,but the plane of the dxy orbital is perpendicular to the direction of the ferroelectric polarization,which hardly suppresses the occurrence of ferroelectricity.Therefore,the multiferroic exits in the CrNCl_(2).In addition,like CrNCl_(2),the CrNBr_(2) is an intrinsic multiferroic with antiferromagneticferroelectric ground state while CrNI_(2) is an intrinsic multiferroic with ferromagnetic-ferroelectric ground state.These findings enrich the multiferroics in the two-dimensional system and enable a wide range of applications in nanoscale devices.展开更多
Electronic, elastic and piezoelectric properties of two-dimensional （2D） group-IV buckled monolayers （GeSi, SnSi and SnGe） are studied by first principle calculations. According to our calculations, SnSi and SnGe ...Electronic, elastic and piezoelectric properties of two-dimensional （2D） group-IV buckled monolayers （GeSi, SnSi and SnGe） are studied by first principle calculations. According to our calculations, SnSi and SnGe are good 2D piezoelectric materials with large piezoelectric coefficients. The values of d11d11 of SnSi and SnGe are 5.04pm/V and 5.42pm/V, respectively, which are much larger than 2D MoS2 （3.6pm/V） and are comparable with some frequently used bulk materials （e.g., wurtzite AlN 5.1pm/V）. Charge transfer is calculated by the L wdin analysis and we find that the piezoelectric coefficients （d11d11 and d31） are highly dependent on the polarizabilities of the anions and cations in group-IV monolayers.展开更多
Using first-principles calculations,hydrogen evolution reaction(HER) activity on two-dimensional(2 D) gallium chalcogenides monolayers GaX(X=O,S,Se,and Te) as well as the derived Janus monolayers Ga_(2) XY(X≠Y,X/Y=O,...Using first-principles calculations,hydrogen evolution reaction(HER) activity on two-dimensional(2 D) gallium chalcogenides monolayers GaX(X=O,S,Se,and Te) as well as the derived Janus monolayers Ga_(2) XY(X≠Y,X/Y=O,S,Se,and Te) were systematically examined.It was found that Ga_(2) OSe Janus monolayer with a 0.3% strain has the lowest ΔG_(H)*of 0.19 eV(modified to-0.01 eV including the solvation effect) because(ⅰ) O is the most electronegative among X/Y atoms,(ⅱ) the Ga_(2) OSe monolayer has a larger lattice parameter with respect to GaO monolayer,and(ⅲ) the built-in electric field is enhanced after H adsorption.The enhanced H adsorption with the lattice stretching is a result of the weaker Ga-O bond strength before H adsorption and the reduced electron fillings of anti-bonding molecular orbital formed by H 1 s and O2 p_(z) orbitals after H adsorption.The O-p_(z) band center can be served as a descriptor to describe the HER activity trend for these p-block materials.Moreover,Ga_(2) OSe monolayer has appropriate band alignment,distinguished optical absorption coefficient(10~5 cm^(-1)),low exciton binding energy(0.71 eV),and the spontaneous HER process,indicating that it is a highly potential candidate for near-infrared photocatalyst for hydrogen production.Our research provides a novel paradigm that forming Janus structure can effectively tune the HER activity,which would guide the searching for excellent HER photocatalysts for clean hydrogen production.展开更多
We study theoretically the exciton Bose–Einstein condensation and exciton vortices in a two-dimensional(2 D)perovskite(PEA)2 Pb I4 monolayer.Combining the first-principles calculations and the Keldysh model,the excit...We study theoretically the exciton Bose–Einstein condensation and exciton vortices in a two-dimensional(2 D)perovskite(PEA)2 Pb I4 monolayer.Combining the first-principles calculations and the Keldysh model,the exciton binding energy of in a(PEA)2 Pb I4 monolayer can approach hundreds of me V,which make it possible to observe the excitonic effect at room temperature.Due to the large exciton binding energy,and hence the high density of excitons,we find that the critical temperature of the exciton condensation could approach the liquid nitrogen regime.In the presence of perpendicular electric fields,the dipole-dipole interaction between excitons is found to drive the condensed excitons confined in(PEA)2 Pb I4 monolayer flakes into patterned vortices,as the evolution time of vortex patterns is comparable to the exciton lifetime.展开更多
Organometallic nanosheets are a versatile platform for design of efficient electrocatalyst materials due to their high surface area and uniform dispersion of metal active sites.In this paper,we systematically investig...Organometallic nanosheets are a versatile platform for design of efficient electrocatalyst materials due to their high surface area and uniform dispersion of metal active sites.In this paper,we systematically investigate the electrocatalytic performance of the first transition metal series TM3–C12S12 monolayers on CO_(2)using spin-polarized density functional theory.The calculations show that M3–C12S12 exhibits excellent catalytic activity and selectivity in the catalytic reduction in CO_(2).The main reduction products of Sc,Ti,and Cr are CH4.V,Mn,Fe and Zn mainly produce HCOOH,and Co produces HCHO,while CO is the main product for Ni and Cu.For Sc,Ti,and Cr,the overpotentials are>0.7 V,while for V,Mn,Fe,Co,Ni,Cu,Zn,the overpotentials are very low and range from 0.27 to 0.47 V.Therefore,our results indicate that many of the M3–C12S12 monolayers are expected to be excellent and efficient CO_(2)reduction catalysts.展开更多
We studied and compared the transport properties of charge carriers in bilayer graphene, monolayer graphene, and the conventional semiconductors （the two-dimensional electron gas （2DEG））. It is elucidated that the...We studied and compared the transport properties of charge carriers in bilayer graphene, monolayer graphene, and the conventional semiconductors （the two-dimensional electron gas （2DEG））. It is elucidated that the normal incidence transmission in the bilayer graphene is identical to that in the 2DEG but totally different from that in the monolayer graphene. However, resonant peaks appear in the non-normal incidence transmission profile for a high barrier in the bilayer graphene, which do not occur in the 2DEG. Furthermore, there are tunneling and forbidden regions in the transmission spectrum for each material, and the division of the two regions has been given in the work. The tunneling region covers a wide range of the incident energy for the two graphene systems, but only exists under specific conditions for the 2DEG. The counterparts of the transmission in the conductance profile are also given for the three materials, which may be used as high-performance devices based on the bilayer graphene.展开更多
Vibrational mode in a two-dimensional dust monolayer is investigated by considering the finite size of dust grains. Each dust grain is assumed to be a negative point charge and a dipole moment due to the inhomogeneous...Vibrational mode in a two-dimensional dust monolayer is investigated by considering the finite size of dust grains. Each dust grain is assumed to be a negative point charge and a dipole moment due to the inhomogeneous charge distribution on its surface. The dispersion relation of the vibrational mode is derived. Both the self-excited and externally excited cases are discussed. It is shown that the mode is sensitive to the direction of the dipole moment.展开更多
The two-dimensional(2D)ferromagnetic materials and the related van der Waals homostructures have attracted considerable interest,while the 2D antiferromagnetic material has not yet been reported.Based on first-princip...The two-dimensional(2D)ferromagnetic materials and the related van der Waals homostructures have attracted considerable interest,while the 2D antiferromagnetic material has not yet been reported.Based on first-principles calculations,we investigate both electronic structures and magnetic orderings of bulk and monolayer of chromium diiodides(CrI2).We demonstrate a counter-intuitive fact that the ground state of the free-standing monolayer of CrI2 is antiferromagnetic though the bulk possesses macroscopic ferromagnetic ordering.The interlayer interaction remains antiferromagnetic up to few-layer scenarios.The unique feature of CrI2 makes it an ideal workbench to investigate the relation between magnetic couplings and interlayer van der Waals interactions,and may offer an opportunity to 2D antiferromagnetic spintronic devices.展开更多
Two-dimensional(2D)ferroelectric compounds are a special class of materials that meet the need for devices miniaturization,which can lead to a wide range of applications.Here,we investigate ferroelectric properties of...Two-dimensional(2D)ferroelectric compounds are a special class of materials that meet the need for devices miniaturization,which can lead to a wide range of applications.Here,we investigate ferroelectric properties of monolayer group-IV monochalcogenides MX(M=Sn,Ge;X=Se,Te,S)via strain engineering,and their effects with contaminated hydrogen are also discussed.GeSe,GeTe,and GeS do not go through transition up to the compressive strain of-5%,and consequently have good ferroelectric parameters for device applications that can be further improved by applying strain.According to the calculated ferroelectric properties and the band gaps of these materials,we find that their band gap can be adjusted by strain for excellent photovoltaic applications.In addition,we have determined the most stable hydrogen occupancy location in the monolayer SnS and SnTe.It reveals that H prefers to absorb on SnS and SnTe monolayers as molecules rather than atomic H.As a result,hydrogen molecules have little effect on the polarization and electronic structure of monolayer SnTe and SnS.展开更多
基金This work was supported by the Excellent Scientist Program of South China University of Technology (324-D60090), the Scientific Research Foundation for the Returned Overseas Chinese Scholars, State Education Ministry (B09-B7060040) and the National Natural Science Foundation of China (20643001)
文摘We describe in this paper the fabrication of two- and one-dimensional nanostructures with organic molecular beam epitaxy （OMBE） principle based on controlled selfassembly by using adsorbate-substrate and intennolecular interactions that are important in molecular fabrication. Cu（100） single crystal was used as substrate in fabricating molecular nanostructures. Scanning tunneling microscopy （STM） experiments confirmed that Zn-tetra- [3,5-di-t-butylphenyl]porphyrin-molecules can be used to fabricate both monolayer and molecular wire on Cu（100） surface simultaneously, and the latter is arranged on the terrace edges. We herein briefly discuss the selectivity in terms of a mechanism in which the highest occupied and lowest unoccupied molecular orbitals （HOMO and LUMO） of the molecules interact with the surface.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11374033,11774030,51735001 and 61775016the Fundamental Research Funds for the Central Universities under Grant No 2017CX10007
文摘We investigate the electronic-transport properties of two-dimensional monolayer films from Au-P-Au molecular junction to Au-Si-Au molecular junction using elastic scattering Green＇s function theory. In the process of replacing the P atoms with Si atoms every other line from the middle of monolayer blue phosphorus molecular structure, the substitution of Si atoms changes the properties of Au-P-Au molecular junction significantly. Interestingly, the current value has a symmetric change as a parabolic curve with the peak appearing in Au-Si_1P_1-Au molecular junction, which provides the most stable current of 15.00 nA in a wide voltage range of 0.70-2.70 V.Moreover, the current-voltage characteristics of the structures indicate that the steps tend to disappear revealing the property similar to metal when the Si atoms dominate the molecular junction.
基金supported by the National Natural Science Foundation of China(22273045,52488101 and 22472043)Ningbo Youth Science and Technology Innovation Leading Talent(2023QL041)Tsinghua University Independent Scientific Research Plan for Young Investigator,Tsinghua University Dushi Program,and Initiative Scientific Research Program。
文摘Directly correlating the morphology and composition of interfacial water is vital not only for studying water icing under critical conditions but also for understanding the role of protein–water interac-tions in bio-relevant systems.In this study,we present a model system to study two-dimensional(2D)water layers under ambient conditions by using self-assembled monolayers(SAMs)supporting the physisorp-tion of the Cytochrome C(Cyt C)protein layer.We observed that the 2D island-like water layers were uniformly distributed on the SAMs as characterized by atomic force microscopy,and their composition was confirmed by nano-atomic force microscopy-infrared spectroscopy and Raman spectroscopy.In addition,these 2D flakes could grow under high-humidity conditions or melt upon the introduction of a heat source.The formation of these flakes is attributed to the activation energy for water desorption from the Cyt C being nearly twofold high than that from the SAMs.Our results provide a new and effective method for further understanding the water–protein interactions.
基金support from the National Natural Science Foundation of China(Grant Nos.12334014 and 11727902)the Overseas High-level Talents Program of the Chinese Academy of Sciences.
文摘We report the discovery of bistable polar states with switchable polarization in the Janus monolayer 1T-MoSSe,induced by symmetry breaking in its chalcogen atomic layers.Our results demonstrate that Janus 1T-MoSSe exhibits two out-of-plane bistable polar states with switchable polarization,rather than polarization emerging from a non-polar phase,which represents an unconventional form of ferroelectric-like behavior.First-principles calculations and phenomenological modeling reveal that the inequivalent stacking of sulfur and selenium(S/Se)atoms breaks central inversion symmetry,activating non-degenerate phonon modes at the K-point(K_(2)/K_(3))that drive the structural transformation between metastable d1TS and d1TSe phases.This coupling enables bipolar control of out-of-plane polarization through atomic displacements and charge redistribution,resulting in a polarization change ofΔP≈±0.3μC/cm^(2).The Landau free energy analysis indicates that anharmonic terms and inter-mode coupling generate an asymmetric double-well potential,which is essential for the stabilization of bistable polar states.Molecular dynamics simulations show that the d1TS phase remains stable at high temperatures,whereas the d1TSe phase undergoes an irreversible phase transition near 300 K,accompanied by a Peierls-like distortion of the Mo atomic chain.This transition is driven by differences in electronegativity,atomic radius,and d-p orbital hybridization between S and Se.Our findings establish a theoretical framework for engineering nonlinear responses in two-dimensional(2D)ferroelectrics and suggest that low-energy polarization reversal at room temperature can be achieved through strain or electric-field control,offering promising opportunities for non-volatile memory and piezoelectric sensing applications.
基金financially supported by the Natural Science Funds for Distinguished Young Scholar of Heilongjiang Province(No.JC2018004)the National Natural Science Foundation of China(No.11964024)+2 种基金the“Grassland Talents”project of Inner Mongolia autonomous region(No.12000-12102613)the Young science and technology talents cultivation project of Inner Mongolia University(No.21221505)supported by Harbin Normal University and Beijing Paratera Technology Co.,Ltd。
文摘Green hydrogen production and CO_(2) fixation have been identified as the fundamental techniques for sustainable economy.The open challenge is to develop high performance catalysts for hydrogen evolution reaction(HER)and CO_(2) electroreduction(CO_(2)ER)to valuable chemicals.Under such context,this work reported computational efforts to design promising electrocatalyst for HER and CO_(2)ER based on the swarm-intelligence algorithm.Among the family of transition-metal phosphides(TMPs),Pt_(2)P_(3) monolayer has been identified as excellent bifunctional catalysts due to high stability,excellent conductivity and superior catalytic performance.Different from typical d-block catalysts,p-band center presented by P atoms within Pt_(2)P_(3) monolayer plays the essential role for its reactivity towards HER and CO_(2)ER,underlining the key value of p-electrons in advanced catalyst design and thus providing a promising strategy to further develop novel catalysts made of p-block elements for various energy applications.
基金Project supported by the National Natural Science Foundation of China(Grant No.11574223)the Natural Science Foundation of Jiangsu Province,China(Grant No.BK20150303)the Jiangsu Specially-Appointed Professor Program of Jiangsu Province,China
文摘Two-dimensional （2D） ferromagnetic （FM） materials have great potential for applications in next-generation spin- tronic devices. Since most 2D FM materials come from van der Waals crystals, stabilizing them on a certain substrate without killing the ferromagnetism is still a challenge. Through systematic first-principles calculations, we proposed a new family of 2D FM materials which combines TaX （X= S, Se or Te） monolayer and A1203（0001） substrate. The TaX monolayers provide magnetic states and the A1203（0001） substrate stabilizes the former. Interestingly, the A1203（0001） substrate leads to a metal-to-insulator transition in the TaX monolayers and induces a band gap up to 303 meV. Our study paves the way to explore promising 2D FM materials for practical applications in spintronics devices.
基金supported by the NSFC(12474071)Natural Science Foundation of Shandong Province(ZR2024YQ051,ZR2025QB50)+6 种基金Guangdong Basic and Applied Basic Research Foundation(2025A1515011191)the Shanghai Sailing Program(23YF1402200,23YF1402400)funded by Basic Research Program of Jiangsu(BK20240424)Open Research Fund of State Key Laboratory of Crystal Materials(KF2406)Taishan Scholar Foundation of Shandong Province(tsqn202408006,tsqn202507058)Young Talent of Lifting engineering for Science and Technology in Shandong,China(SDAST2024QTB002)the Qilu Young Scholar Program of Shandong University。
文摘As emerging two-dimensional(2D)materials,carbides and nitrides(MXenes)could be solid solutions or organized structures made up of multi-atomic layers.With remarkable and adjustable electrical,optical,mechanical,and electrochemical characteristics,MXenes have shown great potential in brain-inspired neuromorphic computing electronics,including neuromorphic gas sensors,pressure sensors and photodetectors.This paper provides a forward-looking review of the research progress regarding MXenes in the neuromorphic sensing domain and discussed the critical challenges that need to be resolved.Key bottlenecks such as insufficient long-term stability under environmental exposure,high costs,scalability limitations in large-scale production,and mechanical mismatch in wearable integration hinder their practical deployment.Furthermore,unresolved issues like interfacial compatibility in heterostructures and energy inefficiency in neu-romorphic signal conversion demand urgent attention.The review offers insights into future research directions enhance the fundamental understanding of MXene properties and promote further integration into neuromorphic computing applications through the convergence with various emerging technologies.
基金supported by the National Natural Science Foundation of China (Grant No.11574244 for G.Y.G.)the XJTU Research Fund for AI Science (Grant No.2025YXYC011 for G.Y.G.)the Hong Kong Global STEM Professorship Scheme (for X.C.Z.)。
文摘Compared to the well-studied two-dimensional(2D)ferroelectricity,the appearance of 2D antiferroelectricity is much rarer,where local dipoles from the nonequivalent sublattices within 2D monolayers are oppositely oriented.Using NbOCl_(2) monolayer with competing ferroelectric(FE)and antiferroelectric(AFE)phases as a 2D material platform,we demonstrate the emergence of intrinsic antiferroelectricity in NbOCl_(2) monolayer under experimentally accessible shear strain,along with new functionality associated with electric field-induced AFE-to-FE phase transition.Specifically,the complex configuration space accommodating FE and AFE phases,polarization switching kinetics,and finite temperature thermodynamic properties of 2D NbOCl_(2) are all accurately predicted by large-scale molecular dynamics simulations based on deep learning interatomic potential model.Moreover,room temperature stable antiferroelectricity with low polarization switching barrier and one-dimensional collinear polarization arrangement is predicted in shear-deformed NbOCl_(2) monolayer.The transition from AFE to FE phase in 2D NbOCl_(2) can be triggered by a low critical electric field,leading to a double polarization–electric(P–E)loop with small hysteresis.A new type of optoelectronic device composed of AFE-NbOCl_(2) is proposed,enabling electric“writing”and nonlinear optical“reading”logical operation with fast operation speed and low power consumption.
基金supported by the National Key Research and Development Program of China (Grant Nos.2024YFA1409800 for J.Z.and2024YFA1408603 for Q.Z.)the National Natural Science Foundation of China (Grant Nos.12125408,12334004for J.Z.,and 12174363 for Q.Z.)+1 种基金the Innovation Program for Quantum Science and Technology (Grant No.2021ZD0303306 for J.Z.)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0450101 for J.Z.)。
文摘Electron–hole(e–h)recombination is a fundamental process that governs energy dissipation and device efficiency in semiconductors.In two-dimensional(2D)materials,the formation of tightly bound excitons makes exciton-mediated e–h recombination the dominant decay pathway.In this work,nonradiative e–h recombination within excitons in monolayer MoS2 is investigated using first-principles simulations that combine nonadiabatic molecular dynamics with𝐺𝑊and real-time Bethe–Salpeter equation(BSE)propagation.A two-step process is identified:rapid intervalley redistribution induced by exchange interaction,followed by slower phonon-assisted recombination facilitated by exciton binding.By selectively removing the screened Coulomb and exchange terms from the BSE Hamiltonian,their respective contributions are disentangled—exchange interaction is found to increase the number of accessible recombination pathways,while binding reduces the excitation energy and enhances nonradiative decay.A reduction in recombination lifetime by over an order of magnitude is observed due to the excitonic many-body effects.These findings provide microscopic insights for understanding and tuning exciton lifetimes in 2D transition-metal dichalcogenides.
基金Supported by the National Natural Science Foundation of China under Grant Nos 11225421,11474277,11434010 and 11574305the National Young 1000 Talent Plan
文摘The fundamental momentum conservation requirement q - 0 for the Raman process is relaxed in the nanocrystal- lites （NCs）, and phonons away from the Brillouin-zone center will be involved in the Raman scattering, which is well-known as the phonon confinement effect in NCs. This usually gives a downshift and asymmetric broadening of the Raman peak in various NCs. Recently, the A1 mode of 1L MoS2 NCs is found to exhibit a blue shift and asymmetric broadening toward the high-frequency side [Chem. Soc. Rev. 44 （2015） 2757 and Phys. Rev. B 91 （2015） 195411]. In this work, we carefully check this issue by studying Raman spectra of lL MoS2 NCs prepared by the ion implantation technique in a wide range of ion-implanted dosage. The same confinement coefficient is used for both E＇ and A＇1 modes in 1L MoS2 NCs since the phonon uncertainty in an NC is mainly determined by its domain size. The asymmetrical broadening near the A＇1 and E＇ modes is attributed to the appearance of defect-activated phonons at the zone edge and the intrinsic asymmetrical broadening of the two modes, where the anisotropy of phonon dispersion curves along Г-K and Г- M is also considered. The photoluminescence spectra confirm the formation of small domain size of 1L MoS2 nanocrystallites in the ion-implanted 1L MoS2. This study provides not only an approach to quickly probe phonon dispersion trends of 2D materials away from Г by the Raman scattering of the corresponding NCs, but also a reference to completely understand the confinement effect of different modes in various nanomaterials.
基金Supported by the National Key Research&Development Projects of China under Grant Nos 2016YFA0202300 and 2018FYA0305800the National Natural Science Foundation of China under Grant Nos 61390501,61474141 and 11604373+1 种基金the CAS Pioneer Hundred Talents Programthe Strategic Priority Research Program of Chinese Academy of Sciences under Grant No XDB28000000
文摘We report on the formation of two-dimensional monolayer AgTe crystal on Ag(111)substrates.The samples are prepared in ultrahigh vacuum by deposition of Te on Ag(111)followed by annealing.Using a scanning tunneling microscope(STM)and low electron energy diffraction(LEED),we investigate the atomic structure of the samples.The STM images and the LEED pattern show that monolayer AgTe crystal is formed on Ag(111).Four kinds of atomic structures of AgTe and Ag(111)are observed:(i)flat honeycomb structure,(ii)bulked honeycomb,(iii)stripe structure,(iv)hexagonal structure.The structural analysis indicates that the formation of the different atomic structures is due to the lattice mismatch and relief of the intrinsic strain in the AgTe layer.Our results provide a simple and convenient method to produce monolayer AgTe atomic crystal on Ag(111)and a template for study of novel physical properties and for future quantum devices.
基金Project supported by the National Key R&D Program of China(Grant No.2019YFB1704600)the International Cooperation Research Project of Shenzhen(Grant No.GJHZ20180413182004161)+2 种基金the Hubei Provincial Natural Science Foundation of China(Grant No.2020CFA032)the National Natural Science Foundation of China(Grant No.51805395)the China Scholarship Council(Grant No.201906270142).
文摘Two-dimensional multiferroics,which simultaneously possess ferroelectricity and magnetism in a single phase,are well-known to possess great potential applications in nanoscale memories and spintronics.On the basis of first-principles calculations,a CrNCl_(2) monolayer is reported as an intrinsic multiferroic.The CrNCl_(2) has an antiferromagnetic ground state,with a N´eel temperature of about 88 K,and it exhibits an in-plane spontaneous polarization of 200 pC/m.The magnetic moments of CrNCl_(2) mainly come from the dxy orbital of the Cr cation,but the plane of the dxy orbital is perpendicular to the direction of the ferroelectric polarization,which hardly suppresses the occurrence of ferroelectricity.Therefore,the multiferroic exits in the CrNCl_(2).In addition,like CrNCl_(2),the CrNBr_(2) is an intrinsic multiferroic with antiferromagneticferroelectric ground state while CrNI_(2) is an intrinsic multiferroic with ferromagnetic-ferroelectric ground state.These findings enrich the multiferroics in the two-dimensional system and enable a wide range of applications in nanoscale devices.
基金Supported by the National Natural Science Foundation of China under Grant No 51672208the National Science and Technology Pillar Program during the Twelfth Five-Year Plan Period under Grant No 2012BAD47B02+2 种基金the Sci-Tech Research and Development Program of Shaanxi Province under Grant Nos 2010K01-120,2011JM6010 and 2015JM5183the Shaanxi Provincial Department of Education under Grant No 2013JK0927the SRF for ROCS of SEM
文摘Electronic, elastic and piezoelectric properties of two-dimensional （2D） group-IV buckled monolayers （GeSi, SnSi and SnGe） are studied by first principle calculations. According to our calculations, SnSi and SnGe are good 2D piezoelectric materials with large piezoelectric coefficients. The values of d11d11 of SnSi and SnGe are 5.04pm/V and 5.42pm/V, respectively, which are much larger than 2D MoS2 （3.6pm/V） and are comparable with some frequently used bulk materials （e.g., wurtzite AlN 5.1pm/V）. Charge transfer is calculated by the L wdin analysis and we find that the piezoelectric coefficients （d11d11 and d31） are highly dependent on the polarizabilities of the anions and cations in group-IV monolayers.
基金supported byNational Natural Science Foundation of China no. 21573002 (HY)Natural Science Funds for Distinguished Young Scholar of Anhui Province (1908085J08)。
文摘Using first-principles calculations,hydrogen evolution reaction(HER) activity on two-dimensional(2 D) gallium chalcogenides monolayers GaX(X=O,S,Se,and Te) as well as the derived Janus monolayers Ga_(2) XY(X≠Y,X/Y=O,S,Se,and Te) were systematically examined.It was found that Ga_(2) OSe Janus monolayer with a 0.3% strain has the lowest ΔG_(H)*of 0.19 eV(modified to-0.01 eV including the solvation effect) because(ⅰ) O is the most electronegative among X/Y atoms,(ⅱ) the Ga_(2) OSe monolayer has a larger lattice parameter with respect to GaO monolayer,and(ⅲ) the built-in electric field is enhanced after H adsorption.The enhanced H adsorption with the lattice stretching is a result of the weaker Ga-O bond strength before H adsorption and the reduced electron fillings of anti-bonding molecular orbital formed by H 1 s and O2 p_(z) orbitals after H adsorption.The O-p_(z) band center can be served as a descriptor to describe the HER activity trend for these p-block materials.Moreover,Ga_(2) OSe monolayer has appropriate band alignment,distinguished optical absorption coefficient(10~5 cm^(-1)),low exciton binding energy(0.71 eV),and the spontaneous HER process,indicating that it is a highly potential candidate for near-infrared photocatalyst for hydrogen production.Our research provides a novel paradigm that forming Janus structure can effectively tune the HER activity,which would guide the searching for excellent HER photocatalysts for clean hydrogen production.
基金Supported by the National Key R&D Programme of China(Grant Nos.2017YFA0303400 and 2016YFE0110000)the National Natural Science Foundation of China(Grant Nos.11574303 and 11504366)+1 种基金the Youth Innovation Promotion Association of Chinese Academy of Sciences(Grant No.2018148)the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB28000000)。
文摘We study theoretically the exciton Bose–Einstein condensation and exciton vortices in a two-dimensional(2 D)perovskite(PEA)2 Pb I4 monolayer.Combining the first-principles calculations and the Keldysh model,the exciton binding energy of in a(PEA)2 Pb I4 monolayer can approach hundreds of me V,which make it possible to observe the excitonic effect at room temperature.Due to the large exciton binding energy,and hence the high density of excitons,we find that the critical temperature of the exciton condensation could approach the liquid nitrogen regime.In the presence of perpendicular electric fields,the dipole-dipole interaction between excitons is found to drive the condensed excitons confined in(PEA)2 Pb I4 monolayer flakes into patterned vortices,as the evolution time of vortex patterns is comparable to the exciton lifetime.
基金support from the National Natural Science Foundation of China(21673087 and 21873032)startup fund(2006013118 and 3004013105)from Huazhong University of Science and Technologythe Fundamental Research Funds for the Central Universities(2019kfy R CPY116)
文摘Organometallic nanosheets are a versatile platform for design of efficient electrocatalyst materials due to their high surface area and uniform dispersion of metal active sites.In this paper,we systematically investigate the electrocatalytic performance of the first transition metal series TM3–C12S12 monolayers on CO_(2)using spin-polarized density functional theory.The calculations show that M3–C12S12 exhibits excellent catalytic activity and selectivity in the catalytic reduction in CO_(2).The main reduction products of Sc,Ti,and Cr are CH4.V,Mn,Fe and Zn mainly produce HCOOH,and Co produces HCHO,while CO is the main product for Ni and Cu.For Sc,Ti,and Cr,the overpotentials are>0.7 V,while for V,Mn,Fe,Co,Ni,Cu,Zn,the overpotentials are very low and range from 0.27 to 0.47 V.Therefore,our results indicate that many of the M3–C12S12 monolayers are expected to be excellent and efficient CO_(2)reduction catalysts.
基金the National Natural Science Foundation of China(Grant No.11104156)the Postdoctoral Science Foundation of China(Grant No.2012M510405)+1 种基金the Independent Research and Development Fund of Tsinghua University,China(Grant No.20121087948)the Beijing Key Lab of Fine Ceramics Opening Fund,China(Grant No.2012200110)
文摘We studied and compared the transport properties of charge carriers in bilayer graphene, monolayer graphene, and the conventional semiconductors （the two-dimensional electron gas （2DEG））. It is elucidated that the normal incidence transmission in the bilayer graphene is identical to that in the 2DEG but totally different from that in the monolayer graphene. However, resonant peaks appear in the non-normal incidence transmission profile for a high barrier in the bilayer graphene, which do not occur in the 2DEG. Furthermore, there are tunneling and forbidden regions in the transmission spectrum for each material, and the division of the two regions has been given in the work. The tunneling region covers a wide range of the incident energy for the two graphene systems, but only exists under specific conditions for the 2DEG. The counterparts of the transmission in the conductance profile are also given for the three materials, which may be used as high-performance devices based on the bilayer graphene.
基金supported by National Natural Science Foundation of China (Nos.10175013,10010760807)
文摘Vibrational mode in a two-dimensional dust monolayer is investigated by considering the finite size of dust grains. Each dust grain is assumed to be a negative point charge and a dipole moment due to the inhomogeneous charge distribution on its surface. The dispersion relation of the vibrational mode is derived. Both the self-excited and externally excited cases are discussed. It is shown that the mode is sensitive to the direction of the dipole moment.
基金This work was supported by the National Natural Science Foundation of China(No.11404043)Graduate Research Innovation Project of Chongqing(No.CYS18253).
文摘The two-dimensional(2D)ferromagnetic materials and the related van der Waals homostructures have attracted considerable interest,while the 2D antiferromagnetic material has not yet been reported.Based on first-principles calculations,we investigate both electronic structures and magnetic orderings of bulk and monolayer of chromium diiodides(CrI2).We demonstrate a counter-intuitive fact that the ground state of the free-standing monolayer of CrI2 is antiferromagnetic though the bulk possesses macroscopic ferromagnetic ordering.The interlayer interaction remains antiferromagnetic up to few-layer scenarios.The unique feature of CrI2 makes it an ideal workbench to investigate the relation between magnetic couplings and interlayer van der Waals interactions,and may offer an opportunity to 2D antiferromagnetic spintronic devices.
基金the National Natural Science Foundation of China(NSFC)(Grant No.12074126)the Foundation for Innovative Research Groups of NSFC(Grant No.51621001)the Fundamental Research Funds for the Central Universities(Grant No.2020ZYGXZR076).
文摘Two-dimensional(2D)ferroelectric compounds are a special class of materials that meet the need for devices miniaturization,which can lead to a wide range of applications.Here,we investigate ferroelectric properties of monolayer group-IV monochalcogenides MX(M=Sn,Ge;X=Se,Te,S)via strain engineering,and their effects with contaminated hydrogen are also discussed.GeSe,GeTe,and GeS do not go through transition up to the compressive strain of-5%,and consequently have good ferroelectric parameters for device applications that can be further improved by applying strain.According to the calculated ferroelectric properties and the band gaps of these materials,we find that their band gap can be adjusted by strain for excellent photovoltaic applications.In addition,we have determined the most stable hydrogen occupancy location in the monolayer SnS and SnTe.It reveals that H prefers to absorb on SnS and SnTe monolayers as molecules rather than atomic H.As a result,hydrogen molecules have little effect on the polarization and electronic structure of monolayer SnTe and SnS.
