Could two-dimensional perovskites fundamentally solve the instability of perovskite photovoltaics

The high efficiency and low production cost enable the halide perovskite solar cells as a promising technology for the next generation photovoltaics.Nevertheless,the relatively poor stability of the organic–inorganic halide perovskites hinders their commercial applications.In the past few years,two-dimensional(2D)perovskite has emerged as a more stable alternative to the three-dimensional(3D)counterparts and attracted intense research interests.Although many attempts and advances have been made,it is still ambiguous that whether the 2D perovskites could bring closure to the stability issue.To answer this essential question,a systematic study of the nature of 2D halide perovskites is necessary.Here,we focus on the stability investigations of 2D perovskites from different perspectives,especially light,heat,ion migration and strain.Several remaining challenges and opening problems are also discussed.With further material and device engineering,we believe that the 2D perovskites would promote perovskite solar cells to a promising future.

Tuning exciton dynamics by the dielectric confinement effect in quasi-two-dimensional perovskites

The dielectric confinement effect plays an essential role in optoelectronic devices.Existing studies on the relationship between the dielectric confinement and the photoelectric properties are inadequate.Herein,three organic spacers with different dielectric constants are employed to tune the exciton dynamics of quasi-two-dimensional(quasi-2D)Ruddlesden–Popper perovskite films.Femtosecond transient absorption spectroscopy reveals that the small dielectric constant ligand enables a weak dynamic disorder and a large modulation depth of the coherent phonons,resulting in a more complete energy transfer and the inhibition of a trap-mediated nonradiative recombination.Additionally,the increase in the bulk-ligand dielectric constant reduces the corresponding exciton binding energy and then suppresses the Auger recombination,which is beneficial for high-luminance lightemitting diodes.This work emphasizes the importance of dielectric confinement for regulating the exciton dynamics of layered perovskites.

Optical properties of two-dimensional perovskites

The optical properties of two-dimensional(2D)perovskites recently receive numerous research focus thanks to the strong quantum and dielectric confinement effects.In addition to the strong excitonic effect at room temperature,2D perovskites also have appealing features that their optical properties can be flexibly tuned by alternating organic or inorganic layers.Particularly,2D chiral perovskites and 2D perovskites based heterostructures are emerging as new platforms to extend their functionalities.To optimize performance of 2D perovskites-based optoelectronic devices,it is critical to understand the fundamentals and explore the strategies to engineer their optical properties.This review begins with an introduction to the excitons and self-trapped excitons of 2D perovskites.Subsequently,inorganic/organic layer effects on optical properties and 2D perovskites based heterostructures are discussed.We also discussed the nonlinear optical properties of 2D perovskite.We are looking forward to that this review can stimulate more efforts to understand and optimize the optical properties of 2D perovskites.

Influence of Organic Cations on the Crystal and Electronic Structures of Two-dimensional Lead Iodide Perovskites

The crystal structures and electronic structures(including band gap,project density of states,partial charge density,effective mass and electron localization function)of the 2D lead iodide perovskites hybrids with different organic spacer cations of 4-fluorophenylethanaminium(4F-PEA^(+)),ethanolamine(EA^(+)),thienylethylamine(TEA^(+))were investigated using first-principles calculations.It was found the higher dipole moment,the stronger the hydrogen bonding between the organic amino and iodide in the inorganic layer,and the larger the[PbI_(6)]^(4-)octahedral distortions in these crystal structure.Further quantifying the degree of the distortions using OctaDist software showed that the distortion of adjacent[PbI_(6)]^(4-)octahedra had a decisive effect on the band gap.Specifically,the greater deviation of Pb-I-Pb bond angles from 180°,together with the larger distortion of multiple[PbI_(6)]^(4-)octahedron resulted in a wider band gap,which was verified by calculated band gap using different DFT methods.The results outlined the relationships of hydrogen bonding,ocathedra distortion and band structure in 2D perovskites,highlighting the importance of the cations on the structural tuning and optoelectronic properties.

High-performance flexible perovskite photodetectors based on single-crystal-like two-dimensional Ruddlesden-Popper thin films

Two-dimensional Ruddlesden-Popper(2DRP)perovskites have attracted intense research interest for optoelectronic applications,due to their tunable optoelectronic properties and better environmental stability than their threedimensional counterparts.Furthermore,high-performance photodetectors based on single-crystal and polycrystalline thin-films 2DRP perovskites have shown great potential for practical application.However,the complex growth process of single-crystal membranes and uncontrollable phase distribution of polycrystalline films hinder the further development of 2DRP perovskites photodetectors.Herein,we report a series of high-performance photodetectors based on single-crystal-like phase-pure 2DRP perovskite films by designing a novel spacer source.Experimental and theoretical evidence demonstrates that phase-pure films substantially suppress defect states and ion migration.These highly sensitive photodetectors show I_(light)/I_(dark) ratio exceeding 3×10^(4),responsivities exceeding 16 A/W,and detectivities exceeding 3×10^(13) Jones,which are higher at least by 1 order than those of traditional mixed-phase thinfilms 2DRP devices(close to the reported single-crystal devices).More importantly,this strategy can significantly enhance the operational stability of optoelectronic devices and pave the way to large-area flexible productions.

Ternary solvent boosts two-dimensional perovskites

In the past few years,organic–inorganic/inorganic lead halide perovskites,most notably CH3NH3Pb I3and its mixed cation/anion compounds,have attracted tremendous research interests in a wide range of different disciplines,which is largely initialized by their unprecedented success in low-cost and highly efficient solar cells.With certified efficiencies of over 22%in the lab-scale devices,

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.

Multiple Hydrogen Bond-Induced Structural Distortion for Broadband White-Light Emission in Two-Dimensional Perovskites

Low-dimensional hybrid lead-halide perovskites with broadband white-light emission upon near-UV excitation have attracted immense scientific interest due to their potential application for the next generation of solid-state lighting as well as scintillators for radiation detection.Recently,broadband emission material is mostly reported in structural distorted perovskites.However,it is still unclear how to generate structural distortion in low-dimensional perovskites.

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.

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.

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.

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.

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.

Single-cell manipulation by two-dimensional micropatterning

Cells are highly sensitive to their geometrical and mechanical microenvironment that directly regulate cell shape,cytoskeleton and organelle,as well as the nucleus morphology and genetic expression.The emerging two-dimensional micropatterning techniques offer powerful tools to construct controllable and well-organized microenvironment for single-cell level investigations with qualitative analysis,cellular standardization,and in vivo environment mimicking.Here,we provide an overview of the basic principle and characteristics of the two most widely-used micropatterning techniques,including photolithographic micropatterning and soft lithography micropatterning.Moreover,we summarize the application of micropatterning technique in controlling cytoskeleton,cell migration,nucleus and gene expression,as well as intercellular communication.

Magnetic proximity effect in the two-dimensional ε-Fe_(2)O_(3)/NbSe_(2)heterojunction

Two-dimensional(2D)magnet/superconductor heterostructures can promote the design of artificial materials for exploring 2D physics and device applications by exotic proximity effects.However,plagued by the low Curie temperature and instability in air,it is hard to realize practical applications for the reported layered magnetic materials at present.In this paper,we developed a space-confined chemical vapor deposition method to synthesize ultrathin air-stable ε-Fe_(2)O_(3) nanosheets with Curie temperature above 350 K.The ε-Fe_(2)O_(3)/NbSe_(2) heterojunction was constructed to study the magnetic proximity effect on the superconductivity of the NbSe_(2) multilayer.The electrical transport results show that the subtle proximity effect can modulate the interfacial spin–orbit interaction while undegrading the superconducting critical parameters.Our work paves the way to construct 2D heterojunctions with ultrathin nonlayered materials and layered van der Waals(vdW)materials for exploring new physical phenomena.

Thermochemical splitting of CO_(2) on perovskites for CO production: A review

Energy supply dominated by fossil energy has been and remains the main cause of carbon dioxide emissions,the major greenhouse gas leading to the current grave climate change challenges.Many technical pathways have been proposed to address the challenges.Carbon capture and utilization(CCU) represents one of the approaches and thermochemical CO_(2) splitting driven by thermal energy is a subset of the CCU,which converts the captured CO_(2) into CO and makes it possible to achieve closed-loop carbon recirculation.Redox-active catalysts are among the most critical components of the thermochemical splitting cycles and perovskites are regarded as the most promising catalysts.Here we review the latest advancements in thermochemical cycles based on perovskites,covering thermodynamic principles,material modifications,reaction kinetics,oxygen pressure control,circular strategies,and demonstrations to provide a comprehensive overview of the topical area.Thermochemical cycles based on such materials require the consideration of trade-off between cost and efficiency,which is related to actual material used,operation mode,oxygen removal,and heat recovery.Lots of efforts have been made towards improving reaction rates,conversion efficiency and cycling stability,materials related research has been lacking-a key aspect affecting the performance across all above aspects.Double perovskites and composite perovskites arise recently as a potentially promising addition to material candidates.For such materials,more effective oxygen removal would be needed to enhance the overall efficiency,for which thermochemical or electrochemical oxygen pumps could contribute to efficient oxygen removal as well as serve as means for inert gas regeneration.The integration of thermochemical CO_(2) splitting process with downstream fuel production and other processes could reduce costs and increase efficiency of the technology.This represents one of the directions for the future research.

Stacking-dependent exchange bias in two-dimensional ferromagnetic/antiferromagnetic bilayers

A clear microscopic understanding of exchange bias is crucial for its application in magnetic recording, and further progress in this area is desired. Based on the results of our first-principles calculations and Monte Carlo simulations,we present a theoretical proposal for a stacking-dependent exchange bias in two-dimensional compensated van der Waals ferromagnetic/antiferromagnetic bilayer heterostructures. The exchange bias effect emerges in stacking registries that accommodate inhomogeneous interlayer magnetic interactions between the ferromagnetic layer and different spin sublattices of the antiferromagnetic layer. Moreover, the on/off switching and polarity reversal of the exchange bias can be achieved by interlayer sliding, and the strength can be modulated using an external electric field. Our findings push the limits of exchange bias systems to extreme bilayer thickness in two-dimensional van der Waals heterostructures, potentially stimulating new experimental investigations and applications.