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.

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.

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.

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.

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.

Image segmentation of exfoliated two-dimensional materials by generative adversarial network-based data augmentation

Mechanically cleaved two-dimensional materials are random in size and thickness.Recognizing atomically thin flakes by human experts is inefficient and unsuitable for scalable production.Deep learning algorithms have been adopted as an alternative,nevertheless a major challenge is a lack of sufficient actual training images.Here we report the generation of synthetic two-dimensional materials images using StyleGAN3 to complement the dataset.DeepLabv3Plus network is trained with the synthetic images which reduces overfitting and improves recognition accuracy to over 90%.A semi-supervisory technique for labeling images is introduced to reduce manual efforts.The sharper edges recognized by this method facilitate material stacking with precise edge alignment,which benefits exploring novel properties of layered-material devices that crucially depend on the interlayer twist-angle.This feasible and efficient method allows for the rapid and high-quality manufacturing of atomically thin materials and devices.

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.

Two-Dimensional Materials for Highly Efficient and Stable Perovskite Solar Cells

Perovskite solar cells(PSCs)offer low costs and high power conversion efficiency.However,the lack of long-term stability,primarily stemming from the interfacial defects and the sus-ceptible metal electrodes,hinders their practical application.In the past few years,two-dimensional(2D)materials(e.g.,graphene and its derivatives,transitional metal dichalcogenides,MXenes,and black phosphorus)have been identified as a promising solution to solving these problems because of their dangling bond-free surfaces,layer-dependent electronic band structures,tunable functional groups,and inherent compactness.Here,recent progress of 2D material toward efficient and stable PSCs is summarized,including its role as both interface materials and electrodes.We discuss their beneficial effects on perovskite growth,energy level alignment,defect passivation,as well as blocking external stimulus.In particular,the unique properties of 2D materials to form van der Waals heterojunction at the bottom interface are emphasized.Finally,perspectives on the further development of PSCs using 2D materials are provided,such as designing high-quality van der Waals heterojunction,enhancing the uniformity and coverage of 2D nanosheets,and developing new 2D materials-based electrodes.

Control of light-matter interactions in two-dimensional materials with nanoparticle-on-mirror structures

Light–matter interactions in two-dimensional(2D)materials have been the focus of research since the discovery of graphene.The light–matter interaction length in 2D materials is,however,much shorter than that in bulk materials owing to the atomic nature of 2D materials.Plasmonic nanostructures are usually integrated with 2D materials to enhance the light–matter interactions,offering great opportunities for both fundamental research and technological applications.Nanoparticle-on-mirror(NPo M)structures with extremely confined optical fields are highly desired in this aspect.In addition,2D materials provide a good platform for the study of plasmonic fields with subnanometer resolution and quantum plasmonics down to the characteristic length scale of a single atom.A focused and up-to-date review article is highly desired for a timely summary of the progress in this rapidly growing field and to encourage more research efforts in this direction.In this review,we will first introduce the basic concepts of plasmonic modes in NPo M structures.Interactions between plasmons and quasi-particles in 2D materials,e.g.,excitons and phonons,from weak to strong coupling and potential applications will then be described in detail.Related phenomena in subnanometer metallic gaps separated by 2D materials,such as quantum tunneling,will also be touched.We will finally discuss phenomena and physical processes that have not been understood clearly and provide an outlook for future research.We believe that the hybrid systems of2D materials and NPo M structures will be a promising research field in the future.

Two-dimensional Cr_(2)Cl_(3)S_(3) Janus magnetic semiconductor with large magnetic exchange interaction and high-T_(C)

The two-dimensional(2D)Janus monolayers are promising in spintronic device application due to their enhanced magnetic couplings and Curie temperatures.Van der Waals CrCl_(3) monolayer has been experimentally proved to have an in-plane magnetic easy axis and a low Curie temperature of 17 K,which will limit its application in spintronic devices.In this work,we propose a new Janus monolayer Cr_(2)Cl_(3)S_(3) based on the first principles calculations.The phonon dispersion and elastic constants confirm that Janus monolayer Cr_(2)Cl_(3)S_(3) is dynamically and mechanically stable.Our Monte Carlo simulation results based on magnetic exchange constants reveal that Janus monolayer Cr_(2)Cl_(3)S_(3) is an intrinsic ferromagnetic semiconductor with TC of 180 K,which is much higher than that of CrCl_(3) due to the enhanced ferromagnetic coupling caused by S substitution.Moreover,the magnetic easy axis of Janus Cr_(2)Cl_(3)S_(3) can be tuned to the perpendicular direction with a large magnetic anisotropy energy(MAE)of 142eV/Cr.Furthermore,the effect of biaxial strain on the magnetic property of Janus monolayer Cr_(2)Cl_(3)S_(3) is evaluated.It is found that the Curie temperature is more robust under tensile strain.This work indicates that the Janus monolayer Cr_(2)Cl_(3)S_(3) presents increased Curie temperature and out-of-plane magnetic easy axis,suggesting greater application potential in 2D spintronic devices.

Dynamic behavior of tunneling triboelectric charges in two-dimensional materials

Although the research history of triboelectrification has been more than 2000 years, there are still many problems to be solved so far.The use of scanning probe microscopy provides an important way to quantitatively study the transfer, accumulation, and dissipation of triboelectric charges in the process of triboelectrification. Two-dimensional materials are considered to be key materials for new electronic devices in the post-Moore era due to their atomic-scale size advantages. If the electrostatic field generated by triboelectrification can be used to replace the traditional gate electrostatic field, it is expected to simplify the structure of two-dimensional electronic devices and reconfigure them at any time according to actual needs. Here, we investigate the triboelectrification process of various two-dimensional materials such as MoS_(2), WSe_(2),and ZnO. Different from traditional bulk materials, after two-dimensional materials are rubbed, the triboelectric charges generated may tunnel through the two-dimensional materials to the underlying substrate surface. Because the tunneling triboelectric charge is protected by the twodimensional material, its stable residence time on the substrate surface can reach more than 7 days, which is more than tens of minutes for the traditional triboelectric charge. In addition, the electrostatic field generated by the tunneling triboelectric charge can effectively regulate the carrier transport performance of two-dimensional materials, and the source–drain current of the field effect device regulated by the triboelectric floating gate is increased by nearly 60 times. The triboelectric charge tunneling phenomenon in two-dimensional materials is expected to be applied in the fields of new two-dimensional electronic devices and reconfigurable functional circuits.

Radiofrequency sensing systems based on emerging two-dimensional materials and devices

As one of the most promising platforms for wireless communication,radiofrequency(RF)electronics have been widely advocated for the development of sensing systems.In particular,monolayer and few-layer two-dimensional(2D)materials exhibiting extraordinary electrical properties not only can be integrated to improve the performance of RF circuits,but also to display exceptional sensing capabilities.This review provides an in-depth perspective of current trends and challenges in the application of 2D materials for RF biochemical sensing,including:(i)theoretical bases to achieve different sensing schemes;(ii)unique properties of 2D materials for reasoning their applications in RF sensing;(iii)developments in 2D RF sensors to facilitate the practice of biochemical sensors with ever-demanding sensitivities,as well as their potential uses in meeting the requirements and challenges of biochemical sensors in the Internet-of-Things era.

Two-dimensional nanomaterials confined single atoms: New opportunities for environmental remediation

Two-dimensional(2D)supports confined single-atom catalysts(2D SACs)with unique geometric and electronic structures have been attractive candidates in different catalytic applications,such as energy conversion and storage,value-added chemical synthesis and environmental remediation.However,their environmental appli-cations lack of a comprehensive summary and in-depth discussion.In this review,recent progresses in synthesis routes and advanced characterization techniques for 2D SACs are introduced,and a comprehensive discussion on their applications in environmental remediation is presented.Generally,2D SACs can be effective in catalytic elimination of aqueous and gaseous pollutants via radical or non-radical routes and transformation of toxic pollutants into less poisonous species or highly value-added products,opening a new horizon for the contami-nant treatment.In addition,in-depth reaction mechanisms and potential pathways are systematically discussed,and the relationship between the structure-performance is highlighted.Finally,several critical challenges within this field are presented,and possible directions for further explorations of 2D SACs in environmental remediation are suggested.Although the research of 2D SACs in the environmental application is still in its infancy,this review will provide a timely summary on the emerging field,and would stimulate tremendous interest for designing more attractive 2D SACs and promoting their wide applications.

Experimental and theoretical studies on two-dimensional vanadium carbide hybrid nanomaterials derived from V_(4)AlC_(3) as excellent catalyst for MgH_(2)

Hydrogen is considered one of the most ideal future energy carriers.The safe storage and convenient transportation of hydrogen are key factors for the utilization of hydrogen energy.In the current investigation,two-dimensional vanadium carbide(VC) was prepared by an etching method using V_(4)AlC_(3) as a precursor and then employed to enhance the hydrogen storage properties of MgH_(2).The studied results indicate that VC-doped MgH_(2) can absorb hydrogen at room temperature and release hydrogen at 170℃. Moreover,it absorbs 5.0 wt.%of H_(2) within 9.8 min at 100℃ and desorbs 5.0 wt.% of H_(2) within 3.2 min at 300℃.The dehydrogenation apparent activation energy of VC-doped MgH_(2) is 89.3 ± 2.8 kJ/mol,which is far lower than that of additive-free MgH_(2)(138.5 ± 2.4 kJ/mol),respectively.Ab-initio simulations showed that VC can stretch Mg-H bonds and make the Mg-H bonds easier to break,which is responsible for the decrease of dehydrogenation temperature and conducive to accelerating the diffusion rate of hydrogen atoms,thus,the hydrogen storage properties of MgH_(2) are remarkable improved through addition of VC.

Waveguide-integrated optical modulators with two-dimensional materials

Waveguide-integrated optical modulators are indispensable for on-chip optical interconnects and optical computing.To cope with the ever-increasing amount of data being generated and consumed,ultrafast waveguide-integrated optical modulators with low energy consumption are highly demanded.In recent years,two-dimensional(2D)materials have attracted a lot of attention and have provided tremendous opportunities for the development of high-performance waveguide-integrated optical modulators because of their extraordinary optoelectronic properties and versatile compatibility.This paper reviews the state-of-the-art waveguide-integrated optical modulators with 2D materials,providing researchers with the developing trends in the field and allowing them to identify existing challenges and promising potential solutions.First,the concept and fundamental mechanisms of optical modulation with 2D materials are summarized.Second,a review of waveguide-integrated optical modulators employing electro-optic,all-optic,and thermo-optic effects is provided.Finally,the challenges and perspectives of waveguide-integrated modulators with 2D materials are discussed.

Topology Optimization of Sound-Absorbing Materials for Two-Dimensional Acoustic Problems Using Isogeometric Boundary Element Method

In this work,an acoustic topology optimizationmethod for structural surface design covered by porous materials is proposed.The analysis of acoustic problems is performed using the isogeometric boundary elementmethod.Taking the element density of porousmaterials as the design variable,the volume of porousmaterials as the constraint,and the minimum sound pressure or maximum scattered sound power as the design goal,the topology optimization is carried out by solid isotropic material with penalization(SIMP)method.To get a limpid 0–1 distribution,a smoothing Heaviside-like function is proposed.To obtain the gradient value of the objective function,a sensitivity analysis method based on the adjoint variable method(AVM)is proposed.To find the optimal solution,the optimization problems are solved by the method of moving asymptotes(MMA)based on gradient information.Numerical examples verify the effectiveness of the proposed topology optimization method in the optimization process of two-dimensional acoustic problems.Furthermore,the optimal distribution of sound-absorbingmaterials is highly frequency-dependent and usually needs to be performed within a frequency band.

Thermal transport in semiconductor nanostructures, graphene,and related two-dimensional materials

We review experimental and theoretical results on thermal transport in semiconductor nanostructures（multilayer thin films, core/shell and segmented nanowires）, single-and few-layer graphene, hexagonal boron nitride, molybdenum disulfide, and black phosphorus. Different possibilities of phonon engineering for optimization of electrical and heat conductions are discussed. The role of the phonon energy spectra modification on the thermal conductivity in semiconductor nanostructures is revealed. The dependence of thermal conductivity in graphene and related two-dimensional（2 D） materials on temperature, flake size, defect concentration, edge roughness, and strain is analyzed.

The Roadmap of 2D Materials and Devices Toward Chips

Due to the constraints imposed by physical effects and performance degra certain limitations in sustaining the advancement of Moore’s law.Two-dimensional(2D)materials have emerged as highly promising candidates for the post-Moore era,offering significant potential in domains such as integrated circuits and next-generation computing.Here,in this review,the progress of 2D semiconductors in process engineering and various electronic applications are summarized.A careful introduction of material synthesis,transistor engineering focused on device configuration,dielectric engineering,contact engineering,and material integration are given first.Then 2D transistors for certain electronic applications including digital and analog circuits,heterogeneous integration chips,and sensing circuits are discussed.Moreover,several promising applications(artificial intelligence chips and quantum chips)based on specific mechanism devices are introduced.Finally,the challenges for 2D materials encountered in achieving circuit-level or system-level applications are analyzed,and potential development pathways or roadmaps are further speculated and outlooked.

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.

High-precision X-ray characterization for basic materials in modern high-end integrated circuit

Semiconductor materials exemplify humanity's unwavering pursuit of enhanced performance,efficiency,and functionality in electronic devices.From its early iterations to the advanced variants of today,this field has undergone an extraordinary evolution.As the reliability requirements of integrated circuits continue to increase,the industry is placing greater emphasis on the crystal qualities.Consequently,conducting a range of characterization tests on the crystals has become necessary.This paper will examine the correlation between crystal quality,device performance,and production yield,emphasizing the significance of crystal characterization tests and the important role of high-precision synchrotron radiation X-ray topography characterization in semiconductor analysis.Finally,we will cover the specific applications of synchrotron radiation characterization in the development of semiconductor materials.