Magnetic and electronic properties of two-dimensional metal-organic frameworks TM_(3)(C_(2)NH)_(12)

The ferromagnetism of two-dimensional(2D)materials has aroused great interest in recent years,which may play an important role in the next-generation magnetic devices.Herein,a series of 2D transition metal-organic framework materials(TM-NH MOF,TM=Sc-Zn)are designed,and their electronic and magnetic characters are systematically studied by means of first-principles calculations.Their structural stabilities are examined through binding energies and ab-initio molecular dynamics simulations.Their optimized lattice constants are correlated to the central TM atoms.These 2D TM-NH MOF nanosheets exhibit various electronic and magnetic performances owing to the effective charge transfer and interaction between TM atoms and graphene linkers.Interestingly,Ni-and Zn-NH MOFs are nonmagnetic semiconductors(SM)with band gaps of 0.41 eV and 0.61 eV,respectively.Co-and Cu-NH MOFs are bipolar magnetic semiconductors(BMS),while Fe-NH MOF monolayer is a half-semiconductor(HSM).Furthermore,the elastic strain could tune their magnetic behaviors and transformation,which ascribes to the charge redistribution of TM-3d states.This work predicts several new 2D magnetic MOF materials,which are promising for applications in spintronics and nanoelectronics.

The Model for Linear Magnetoresistance of Two-Dimensional Metal-Semiconductor Composites with Interfacial Shells

A metal-semiconductor composite with the interracial shells is investigated theoretically for the large linear mag- netoresistance effect of high doping Ag2＋δ Se and Ag2＋δ te materials. The magnetoresistance （MR） of composites is a function of the magnetic field, temperature, the conductivities of two phases without magnetic field, and the thickness and conductivity of the interracial shells. The MR increases with the increase of the magnetic field and with the decrease of temperature, and no saturation is found even under the high magnetic field. Moreover, it is interestingly found that the interracial shell is an important factor for the MR of the composites. The MR increases with the thickness and the conductivity of the interfacial shells. Lastly, the theoretical results on the MR are compared with the experimental data. It is found that the value of the MR of the composite with the interfacial shell is larger than that without the interfacial shell.

Two-Dimensional Metal-Halide Perovskite-based Optoelectronics: Synthesis, Structure, Properties and Applications

In the past decade, metal-halide perovskites have attracted increasing attention in optoelectronics, due to their superior optoelectronic properties.However, inherent instabilities of conventional three-dimensional(3D)perovskites over moisture, heat, and light remain a severe challenge before the realization of commercial application of metal-halide perovskites.Interestingly, when the dimensions of metal-halide perovskites are reduced to two dimensions(2D), many of the novel properties will arise, such as enlarged bandgap, high photoluminescence quantum yield, and large exciton binding energy. As a result, 2D metal-halide perovskite-based optoelectronic devices display excellent performance, particularly as ambient stable solar cells with excellent power conversion efficiency(PCE), high-performance light-emitting diodes(LEDs) with sharp emission peak, and high-sensitive photodetectors. In this review, we first introduce the synthesis, structure,and physical properties of 2D perovskites. Then, the 2D perovskite-based solar cells, LEDs, and photodetectors are discussed. Finally, a brief overview of the opportunities and challenges for 2D perovskite optoelectronics is presented.

Two-dimensional metal oxide nanosheets for rechargeable batteries

Two-dimensional（2D） metal oxide nanosheets have attracted much attention as potential electrode materials for rechargeable batteries in recent years. This is primarily due to their natural abundance, environmental compatibility, and low cost as well as good electrochemical properties. Despite the fact that most metal oxides possess low conductivity, the introduction of some conductive heterogeneous components, such as nano-carbon, carbon nanotubes（CNTs）, and graphene, to form metal oxide-based hybrids,can effectively overcome this drawback. In this mini review, we will summarize the recent advances of three typical 2D metal oxide nanomaterials, namely, binary metal oxides, ternary metal oxides, and hybrid metal oxides, which are used for the electrochemical applications of next-generation rechargeable batteries, mainly for lithium-ion batteries（LIBs） and sodium-ion batteries（SIBs）. Hence, this review intends to functionalize as a good reference for the further research on 2D nanomaterials and the further development of energy-storage devices.

Ultrathin two-dimensional metal–organic framework nanosheets for efficient electrochemical CO_(2) reduction

Electrochemical CO_(2) reduction into CO or high-value products is regarded as a feasible pathway for energy conversion,which has attracted universal attention in recent years [1-3].However,the reduction of CO_(2) molecule is a thermodynamically uphill process,which involves multiple elemental steps and the competition of hydrogen evolution reaction(HER) in aqueous solution.

Low Frequency Dispersion Law for Two-Dimensional Metallic Photonic Crystals

Using the rigorous multiple-scattering theory, we study the dispersion relation of electromagnetic （EM） waves in two dimensional dielectric photonic crystals （PCs） and metallic photonic crystals （MPCs） in the low-frequency limit. Analytic formula for the effective velocity of EM waves in PCs and MPCs is obtained. Accuracy of our formula is checked by comparing the results with rigorous calculations. For PCs, our result is exactly the same as the coherent potential approximation （CPA）, which is accurate even when the filling fraction is high. But for MPCs, our approach demonstrates special advantages, while the CPA theory fails, in predicting the effective velocity of EM waves in MPCs at low frequency.

Rare π_5~6…Pb Interactions in a Two-dimensional Metal-organic Coordination Polymer with Two Distinct Kinds of Axially Chiral Units

A new metal-organic coordination polymer [Pb（mfpdc）（CH3OH）]n （1, mfpdc = 2,6-dimethyl-4-（2-furanyl） pyridine-3,5-dicarboxylate） was synthesized and characterized by single-crystal X-ray analyses. The crystal is orthorhombic, space group Pbca, a = 15.6297（18）, b = 9.4803（11）, c = 18.598（2） A, V= 2755.8（6） A3, Z = 8, Mr= 498.44, Dc= 2.403 Mg/m3, F（000） = 1872, the final R = 0.0275 and wR = 0.0726 （1 〉 2σ（I））. There are interesting polynuclear zigzag （PbOs）n chains in the structure of 1, and there have interesting axially chiral S- and R-unit Pb4L units constructed from prochiral organic ligands through C-H...O bonding. The （R/S）-Pb4L units by sharing Pb centers generate a 2-D coordination network, in which there exist rare n65Pb （3.2610 A） interactions. The solid-state photoluminescent emission of compound 1 appears at 487 nm.

Two-dimensional metallic behavior at polar MgO/BaTiO_3(110) interfaces

The first-principles calculations are employed to investigate the electrical properties of polar MgO/BaTiO3（110）interfaces. Both n-type and p-type polar interfaces show a two-dimensional metallic behavior. For the n-type polar interface,the interface Ti3d electrons are the origin of the metallic and magnetic properties. Varying the thickness of Ba TiO3 may induce an insulator–metal transition, and the critical thickness is 4 unit cells. For the p-type polar interface, holes preferentially occupy the interface O 2p y state, resulting in a conducting interface. The unbalance of the spin splitting of the O 2p states in the interface Mg O layer leads to a magnetic moment of about 0.25μB per O atom at the interface.These results further demonstrate that other polar interfaces, besides LaAlO3/SrTiO3, can show a two-dimensional metallic behavior. It is helpful to fully understand the role of polar discontinuity on the properties of the interface, which widens the field of polar-nonpolar interfaces.

Recent progress of two-dimensional metal-base catalysts in urea oxidation reaction

Urea oxidation reaction(UOR)is an auxiliary water electrolysis hydrogen production technology developed in recent years to replace oxygen evolution reaction and reduce energy consumption,which can produce hydrogen more efficiently by low theoretical potential,reduce the average cost of electrochemical hydrogen production,and is a frontier research hotspot for renewable hydrogen energy.Two-dimensional(2D)nanomaterials as electrocatalysts have many favorable potential,such as it can effectively reduce the resistivity of materials and increase the specific surface area with certainty.This paper reviews the application of 2D materials in UOR in alkaline electrolytes.And a cross-sectional comparison of various material performance data including overpotential,Tafel slope,electrochemical active surface area(ECSA)and it stability test was conducted,which could illustrate the differences between materials composed of different elements.In addition,the main challenges hindering the progress of research on 2D materials in urea electrocatalysis processes and promising materials in this field in future are summarized and prospected.It is believed that this review will contribute to designing and analyzing highperformance 2D urea electrocatalysts for water splitting.

Emerging two-dimensional Mo-based materials for rechargeable metal-ion batteries:Advances and perspectives

With the rapid development of rechargeable metal-ion batteries(MIBs)with safety,stability and high energy density,significant efforts have been devoted to exploring high-performance electrode materials.In recent years,two-dimensional(2D)molybdenum-based(Mo-based)materials have drawn considerable attention due to their exceptional characteristics,including low cost,unique crystal structure,high theoretical capacity and controllable chemical compositions.However,like other transition metal compounds,Mo-based materials are facing thorny challenges to overcome,such as slow electron/ion transfer kinetics and substantial volume changes during the charge and discharge processes.In this review,we summarize the recent progress in developing emerging 2D Mo-based electrode materials for MIBs,encompassing oxides,sulfides,selenides,carbides.After introducing the crystal structure and common synthesis methods,this review sheds light on the charge storage mechanism of several 2D Mo-based materials by various advanced characterization techniques.The latest achievements in utilizing 2D Mo-based materials as electrode materials for various MIBs(including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)and zinc-ion batteries(ZIBs))are discussed in detail.Afterwards,the modulation strategies for enhancing the electrochemical performance of 2D Mo-based materials are highlighted,focusing on heteroatom doping,vacancies creation,composite coupling engineering and nanostructure design.Finally,we present the existing challenges and future research directions for 2D Mo-based materials to realize high-performance energy storage systems.

Recent progress of two-dimensional metal-organic-frameworks:From synthesis to electrocatalytic oxygen evolution

High-performance electrocatalysts for oxygen evolution reaction(OER)are crucial for water splitting and metal-air batteries.Twodimensional(2D)metal-organic framework(MOF)has become a new class of efficient OER electrocatalysts due to the rich coordination unsaturated metal nodes,large specific surface area,and adjustable structures.In addition,because inheriting the original microstructure of MOFs and having stronger chemical and mechanical stability,metal/alloy/oxide,metal sulfide/selenide/phosphide,and other compounds derived from 2D MOFs have also shown their unique OER catalytic ability.Here,we briefly introduced the existing reaction mechanism and evaluation parameters of catalyst performance of OER,introduced the synthesis methods and corresponding characterization techniques of 2D MOFs and their derivatives,and summarized the latest progress of 2D MOFs and their derivatives as OER catalysts.Finally,we put forward some views and suggestions on the existing problems hindering the development of 2D MOFs as OER for advancing the field.

Alternating spin splitting of electronic and magnon bands in two-dimensional altermagnetic materials

Unconventional antiferromagnetism dubbed as altermagnetism was first discovered in rutile structured magnets,which is featured by spin splitting even without the spin–orbital coupling effect.This interesting phenomenon has been discovered in more altermagnetic materials.In this work,we explore two-dimensional altermagnetic materials by studying two series of two-dimensional magnets,including MF4 with M covering all 3d and 4d transition metal elements,as well as TS2 with T=V,Cr,Mn,Fe.Through the magnetic symmetry operation of RuF4 and MnS2,it is verified that breaking the time inversion is a necessary condition for spin splitting.Based on symmetry analysis and first-principles calculations,we find that the electronic bands and magnon dispersion experience alternating spin splitting along the same path.This work paves the way for exploring altermagnetism in two-dimensional materials.

Progress on two-dimensional ferrovalley materials

The electron's charge and spin degrees of freedom are at the core of modern electronic devices. With the in-depth investigation of two-dimensional materials, another degree of freedom, valley, has also attracted tremendous research interest. The intrinsic spontaneous valley polarization in two-dimensional magnetic systems, ferrovalley material, provides convenience for detecting and modulating the valley. In this review, we first introduce the development of valleytronics.Then, the valley polarization forms by the p-, d-, and f-orbit that are discussed. Following, we discuss the investigation progress of modulating the valley polarization of two-dimensional ferrovalley materials by multiple physical fields, such as electric, stacking mode, strain, and interface. Finally, we look forward to the future developments of valleytronics.

Recent advances in two-dimensional photovoltaic devices

Two-dimensional(2D)materials have attracted tremendous interest in view of the outstanding optoelectronic properties,showing new possibilities for future photovoltaic devices toward high performance,high specific power and flexibility.In recent years,substantial works have focused on 2D photovoltaic devices,and great progress has been achieved.Here,we present the review of recent advances in 2D photovoltaic devices,focusing on 2D-material-based Schottky junctions,homojunctions,2D−2D heterojunctions,2D−3D heterojunctions,and bulk photovoltaic effect devices.Furthermore,advanced strategies for improving the photovoltaic performances are demonstrated in detail.Finally,conclusions and outlooks are delivered,providing a guideline for the further development of 2D photovoltaic devices.

Unlocking the potential of ultra-thin two-dimensional antimony materials:Selective growth and carbon coating for efficient potassium-ion storage

Antimony-based anodes have attracted wide attention in potassium-ion batteries due to their high theoretical specific capacities(∼660 mA h g^(-1))and suitable voltage platforms.However,severe capacity fading caused by huge volume change and limited ion transportation hinders their practical applications.Recently,strategies for controlling the morphologies of Sb-based materials to improve the electrochemical performances have been proposed.Among these,the two-dimensional Sb(2D-Sb)materials present excellent properties due to shorted ion immigration paths and enhanced ion diffusion.Nevertheless,the synthetic methods are usually tedious,and even the mechanism of these strategies remains elusive,especially how to obtain large-scale 2D-Sb materials.Herein,a novel strategy to synthesize 2D-Sb material using a straightforward solvothermal method without the requirement of a complex nanostructure design is provided.This method leverages the selective adsorption of aldehyde groups in furfural to induce crystal growth,while concurrently reducing and coating a nitrogen-doped carbon layer.Compared to the reported methods,it is simpler,more efficient,and conducive to the production of composite nanosheets with uniform thickness(3–4 nm).The 2D-Sb@NC nanosheet anode delivers an extremely high capacity of 504.5 mA h g^(-1) at current densities of 100 mA g^(-1) and remains stable for more than 200 cycles.Through characterizations and molecular dynamic simulations,how potassium storage kinetics between 2D Sb-based materials and bulk Sb-based materials are explored,and detailed explanations are provided.These findings offer novel insights into the development of durable 2D alloy-based anodes for next-generation potassium-ion batteries.

Recent progress on valley polarization and valley-polarized topological states in two-dimensional materials

Valleytronics, using valley degree of freedom to encode, process, and store information, may find practical applications in low-power-consumption devices. Recent theoretical and experimental studies have demonstrated that twodimensional(2D) honeycomb lattice systems with inversion symmetry breaking, such as transition-metal dichalcogenides(TMDs), are ideal candidates for realizing valley polarization. In addition to the optical field, lifting the valley degeneracy of TMDs by introducing magnetism is an efficient way to manipulate the valley degree of freedom. In this paper, we first review the recent progress on valley polarization in various TMD-based systems, including magnetically doped TMDs,intrinsic TMDs with both inversion and time-reversal symmetry broken, and magnetic TMD heterostructures. When topologically nontrivial bands are empowered into valley-polarized systems, valley-polarized topological states, namely valleypolarized quantum anomalous Hall effect can be realized. Therefore, we have also reviewed the theoretical proposals for realizing valley-polarized topological states in 2D honeycomb lattices. Our paper can help readers quickly grasp the latest research developments in this field.

Global dust density in two-dimensional complex plasma

The driven-dissipative Langevin dynamics simulation is used to produce a two-dimensional(2D) dense cloud, which is composed of charged dust particles trapped in a quadratic potential. A 2D mesh grid is built to analyze the center-to-wall dust density. It is found that the local dust density in the outer region relative to that of the inner region is more nonuniform,being consistent with the feature of quadratic potential. The dependences of the global dust density on equilibrium temperature, particle size, confinement strength, and confinement shape are investigated. It is found that the particle size, the confinement strength, and the confinement shape strongly affect the global dust density, while the equilibrium temperature plays a minor effect on it. In the direction where there is a stronger confinement, the dust density gradient is bigger.

Anomalous valley Hall effect in two-dimensional valleytronic materials

The anomalous valley Hall effect(AVHE)can be used to explore and utilize valley degrees of freedom in materials,which has potential applications in fields such as information storage,quantum computing and optoelectronics.AVHE exists in two-dimensional(2D)materials possessing valley polarization(VP),and such 2D materials usually belong to the hexagonal honeycomb lattice.Therefore,it is necessary to achieve valleytronic materials with VP that are more readily to be synthesized and applicated experimentally.In this topical review,we introduce recent developments on realizing VP as well as AVHE through different methods,i.e.,doping transition metal atoms,building ferrovalley heterostructures and searching for ferrovalley materials.Moreover,2D ferrovalley systems under external modulation are also discussed.2D valleytronic materials with AVHE demonstrate excellent performance and potential applications,which offer the possibility of realizing novel low-energy-consuming devices,facilitating further development of device technology,realizing miniaturization and enhancing functionality of them.

Boosting MA-based two-dimensional Ruddlesden-Popper perovskite solar cells by incorporating a binary spacer

Two-dimensional Ruddlesden-Popper(2DRP)perovskite exhibits excellent stability in perovskite solar cells(PSCs)due to introducing hydrophobic long-chain organic spacers.However,the poor charge transporting property of bulky organic cation spacers limits the performance of 2DRP PSCs.Inspired by the Asite cation alloying strategy in 3D perovskites,2DRP perovskites with a binary spacer can promote charge transporting compared to the unary spacer counterparts.Herein,the superior MA-based 2DRP perovskite films with a binary spacer,including 3-guanidinopropanoic acid(GPA)and 4-fluorophenethylamine(FPEA)are realized.These films(GPA_(0.85)FPEA_(0.15))_(2)MA_(4)Pb_5I_(16)show good morphology,large grain size,decreased trap state density,and preferential orientation of the as-prepared film.Accordingly,the present 2DRP-based PSC with the binary spacer achieves a remarkable efficiency of 18.37%with a V_(OC)of1.15 V,a J_(SC)of 20.13 mA cm^(-2),and an FF of 79.23%.To our knowledge,the PCE value should be the highest for binary spacer MA-based 2DRP(n≤5)PSCs to date.Importantly,owing to the hydrophobic fluorine group of FPEA and the enhanced interlayer interaction by FPEA,the unencapsulated 2DRP PSCs based on binary spacers exhibit much excellent humidity stability and thermal stability than the unary spacer counterparts.

Low-frequency hybridized excess vibrations of two-dimensional glasses

One hallmark of glasses is the existence of excess vibrational modes at low frequenciesωbeyond Debye’s prediction.Numerous studies suggest that understanding low-frequency excess vibrations could help gain insight into the anomalous mechanical and thermodynamic properties of glasses.However,there is still intensive debate as to the frequency dependence of the population of low-frequency excess vibrations.In particular,excess modes could hybridize with phonon-like modes and the density of hybridized excess modes has been reported to follow D_(exc)(ω)~ω^(2)in 2D glasses with an inverse power law potential.Yet,the universality of the quadratic scaling remains unknown,since recent work suggested that interaction potentials could influence the scaling of the vibrational spectrum.Here,we extend the universality of the quadratic scaling for hybridized excess modes in 2D to glasses with potentials ranging from the purely repulsive soft-core interaction to the hard-core one with both repulsion and attraction as well as to glasses with significant differences in density or interparticle repulsion.Moreover,we observe that the number of hybridized excess modes exhibits a decrease in glasses with higher density or steeper interparticle repulsion,which is accompanied by a suppression of the strength of the sound attenuation.Our results indicate that the density bears some resemblance to the repulsive steepness of the interaction in influencing low-frequency properties.