Progress in oxygen behaviors in two-dimensional thin films

With the development of spintronics,the investigation on the behavior of oxygen in two-dimensional materials has never ceased.On account of its lively nature,oxygen is hard to exist alone in the system.However,it will interact with other atoms and produce complex orbital hybridization effect,which has influenced the performance of the material.Especially for materials in nanoscale,it is inevitable to introduce the oxygen atoms,no matter what in the process of preparation or employ.Therefore,it is necessary to carry on the research about the effect of oxygen behaviors in the two-dimensional thin films.In this paper,it will mainly introduce the effect of oxygen behaviors on the magnetic properties,electrical properties,phase transition,spin-dependent properties and thermal stability,summarize several factors which influence the oxygen behaviors,and generalize the research progress of the mechanism behind the oxygen behaviors.

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.

Controlled crystal orientation of two-dimensional Ruddlesden-Popper halide perovskite films for solar cells

Metal halide perovskite solar cells have attracted considerable attention because of their high-power conversion efficiency and costeffective solution-processable fabrication;however,they exhibit poor structural stability.Two-dimensional(2D)Ruddlesden-Popper(RP)perovskites could address the aforementioned issue and present excellent stability because of their hydrophobic organic spacer cations.However,the crystallographic orientation of 2D crystals should be perpendicular to the bottom substrates for charges to transport fast and be collected in solar cells.Moreover,controlling the crystallographic orientation of the 2D RP perovskites prepared by the solution process is difficult.Herein,we reviewed the progress of recent research regarding 2D RP perovskite films with the focus on the crystallographic orientation mechanism and orientation controlling methods.Furthermore,the current issues and prospects of 2D RP perovskites in the photovoltaic field were discussed to elucidate their development and application in the future.

Two-dimensional equations for thin-films of ionic conductors

A theoretical model is developed for predicting both conduction and diffusion in thin-film ionic conductors or cables. With the linearized Poisson-Nernst-Planck(PNP)theory, the two-dimensional(2D) equations for thin ionic conductor films are obtained from the three-dimensional(3D) equations by power series expansions in the film thickness coordinate, retaining the lower-order equations. The thin-film equations for ionic conductors are combined with similar equations for one thin dielectric film to derive the 2D equations of thin sandwich films composed of a dielectric layer and two ionic conductor layers. A sandwich film in the literature, as an ionic cable, is analyzed as an example of the equations obtained in this paper. The numerical results show the effect of diffusion in addition to the conduction treated in the literature. The obtained theoretical model including both conduction and diffusion phenomena can be used to investigate the performance of ionic-conductor devices with any frequency.

Photoluminescence Properties of Two-dimensional Planar Layer and Three-dimensional Island Layer for ZnO Films Grown Using MOCVD

ZnO（002） films with different thicknesses ranging from 7 to 300 nm were grown on sapphire（006） substrates via metal-organic chemical vapor deposition （MOCVD）. The two-dimensional（2D） planar layer and the three-dimensional（3D） island layer were studied by using of X-ray diffraction（XRD） rocking curves and atomic force microscopy （AFM）. The room temperature photoluminescence （PL） spectra show a blue shift of the peak positions of the uhraviolet（UV） emission with increasing film thickness. The blue shift is remarkably high（393-380 nm） when an increase in film thickness（7-15 nm） is accompanied by the change of structure from a 2D planar layer to a 3D island layer. The PL spectra at 77 K also indicate that there are different transition mechanisms in the film thickness from a 2D planar layer to a 3D island layer near the 2D layer region.

Electron Transport Properties of Two-Dimensional Monolayer Films from Au-P-Au to Au-Si-Au Molecular Junctions

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.

Critical behavior in the epitaxial growth of two-dimensional tellurium films on SrTiO_(3)(001) substrates

Materials' properties may differ in the thin-film form, especially for epitaxial ultra-thin films, where the substrates play an important role in their deviation from the bulk quality. Here by molecular beam epitaxy(MBE) and scanning tunneling microscopy/spectroscopy, we investigate the growth kinetics of ultra-thin tellurium(Te) films on SrTiO_(3)(STO)(001). The MBE growth of Te films usually exhibits Volmer–Weber(VW) island growth mode and no a-few-monolayer film with full coverage has been reported. The absence of wetting-layer formation in the VW growth mode of Te on STO(001) is resulted from its low diffusion barriers as well as its relatively higher surface energy compared with those of the substrate and the interface. Here we circumvent these limiting factors and achieve the growth of ultra-thin β-Te films with near-complete coverages by driving the growth kinetics to the extreme condition. There is a critical thickness(3 monolayer) above which the two-dimensional Te films can form on the STO(001) substrate. In addition, the scanning tunneling spectra on the ultra-thin Te film grown on STO exhibits an enormously large forbidden gap compared with that grown on the graphene substrate. Our work establishes the necessary conditions for the growth of ultra-thin materials with similar kinetics and thermodynamics.

Significantly Improved High-Temperature Energy Storage Performance of BOPP Films by Coating Nanoscale Inorganic Layer

Biaxially oriented polypropylene(BOPP)is one of the most commonly used commercial capacitor films,but its upper operating temperature is below 105℃due to the sharply increased electrical conduction loss at high temperature.In this study,growing an inorganic nanoscale coating layer onto the BOPP film's surface is proposed to suppress electrical conduction loss at high temperature,as well as increase its upper operating temperature.Four kinds of inorganic coating layers that have different energy band structure and dielectric property are grown onto the both surface of BOPP films,respectively.The effect of inorganic coating layer on the high-temperature energy storage performance has been systematically investigated.The favorable coating layer materials and appropriate thickness enable the BOPP films to have a significant improvement in high-temperature energy storage performance.Specifically,when the aluminum nitride(AIN)acts as a coating layer,the AIN-BOPP-AIN sandwich-structured films possess a discharged energy density of 1.5 J cm^(-3)with an efficiency of 90%at 125℃,accompanying an outstandingly cyclic property.Both the discharged energy density and operation temperature are significantly enhanced,indicating that this efficient and facile method provides an important reference to improve the high-temperature energy storage performance of polymer-based dielectric films.

Photodetectors based on two-dimensional materials and organic thin-film heterojunctions

High-performance photodetectors are expected to open up revolutionary opportunities in many application fields, such as environment monitoring, military, optical communication and biomedical science. Combining two-dimensional materials(which have tunable optical absorption and high carrier mobility) with organic materials(which are abundant with low cost, high flexibility and large-area scalability) to form thin-film heterojunctions, high-responsivity photodetectors could be predicted with fast response speed in a wide spectra region.In this review, we give a comprehensive summary of photodetectors based on two-dimensional materials and organic thin-film heterojunctions, which includes hybrid assisted enhanced devices, single-layer enhanced devices, vertical heterojunction devices and tunable vertical heterojunction devices. We also give a systematic classification and perspectives on the future development of these types of photodetectors.

Flexible, Transparent and Conductive Metal Mesh Films with Ultra‑High FoM for Stretchable Heating and Electromagnetic Interference Shielding

Despite the growing demand for transparent conductive films in smart and wearable electronics for electromagnetic interference(EMI)shielding,achieving a flexible EMI shielding film,while maintaining a high transmittance remains a significant challenge.Herein,a flexible,transparent,and conductive copper(Cu)metal mesh film for EMI shielding is fabricated by self-forming crackle template method and electroplating technique.The Cu mesh film shows an ultra-low sheet resistance(0.18Ω□^(-1)),high transmittance(85.8%@550 nm),and ultra-high figure of merit(>13,000).It also has satisfactory stretchability and mechanical stability,with a resistance increases of only 1.3%after 1,000 bending cycles.As a stretchable heater(ε>30%),the saturation temperature of the film can reach over 110°C within 60 s at 1.00 V applied voltage.Moreover,the metal mesh film exhibits outstanding average EMI shielding effectiveness of 40.4 dB in the X-band at the thickness of 2.5μm.As a demonstration,it is used as a transparent window for shielding the wireless communication electromagnetic waves.Therefore,the flexible and transparent conductive Cu mesh film proposed in this work provides a promising candidate for the next-generation EMI shielding applications.

Two-dimensional analysis of progressive delamination in thin film electrodes

By employing the two-dimensional analysis, i.e.,plane strain and plane stress, a semi-analytical method is developed to investigate the interfacial delamination in electrodes. The key parameters are obtained from the governing equations, and their effects on the evolution of the delamination are evaluated. The impact of constraint perpendicular to the plane is also investigated by comparing the plane strain and plane stress. It is found that the delamination in the plane strain condition occurs easier, indicating that the constraint is harmful to maintain the structure stability. According to the obtained governing equations, a formula of the dimensionless critical size for delamination is provided, which is a function of the maximum volumetric strain and the Poisson’s ratio of the active layer.

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.

Effects of Thickness and Anisotropic Strain on Polarization Switching Properties of Sub-10nm Epitaxial Hf_(0.5)Zr_(0.5)O_(2)Thin Films

Doped HfO_(2)-based ferroelectric(FE)films are emerging as leading contenders for next-generation FE nonvolatile memories due to their excellent compatibility with complementary metal oxide semiconductor processes and robust ferroelectricity at nanoscale dimensions.Despite the considerable attention paid to the FE properties of HfO_(2)-based films in recent years,enhancing their polarization switching speed remains a critical research challenge.We demonstrate the strong ferroelectricity of sub-10nm Hf_(0.5)Zr_(0.5)O_(2)(HZO)thin films and show that the polarization switching speed of these thin films can be significantly affected by HZO thickness and anisotropically strained La_(0.67)Sr_(0.33)MO_(3)-buffered layer.Our observations indicate that the HZO thin film thickness and anisotropically strained La_(0.67)Sr_(0.33)MO_(3)layer influence the nucleation of reverse domains by altering the phase composition of the HZO thin film,thereby reducing the polarization switching time.Although the increase in HZO thickness and anisotropic compressive strain hinder the formation of the FE phase,they can enable faster switching.Our findings suggest that FE HZO ultrathin films with polar orthorhombic structures have broad application prospects in microelectronic devices.These insights into novel methods for increasing polarization switching speed are poised to advance the development of high-performance FE devices.

Centimeter-Scale Above-Room-Temperature Ferromagnetic Fe_(3)GaTe_(2)Thin Films by Molecular Beam Epitaxy

Fe_(3)GaTe_(2),as a layered ferromagnetic material,has a Curie temperature(T_(c))higher than room temperature,making it the key material in next-generation spintronic devices.To be used in practical devices,large-sized high-quality Fe_(3)GaTe_(2)thin films need to be prepared.Here,the centimeter-scale thin film samples with high crystal quality and above-room-temperature ferromagnetism with strong perpendicular magnetic anisotropy were prepared by molecular beam epitaxy technology.Furthermore,the Tc of the samples raises as the film thickness increases,and reaches 367K when the film thickness is 60 nm.This study provides material foundations for the new generation of van der Waals spintronic devices and paves the way for the commercial application of Fe_(3)GaTe_(2).

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.

Ultrathin Limit on the Anisotropic Superconductivity of Single-Layered Cuprate Films

Exploring dimensionality effects on cuprates is important for understanding the nature of high-temperature superconductivity.By atomically layer-by-layer growth with oxide molecular beam epitaxy,we demonstrate that La_(2−x)Sr_(x)CuO_(4)(x=0.15)thin films remain superconducting down to 2 unit cells of thickness but quickly reach the maximum superconducting transition temperature at and above 4 unit cells.By fitting the critical magnetic field(μ0H_(c2)),we show that the anisotropy of the film’s superconductivity increases with decreasing film thickness,indicating that the superconductivity of the film gradually evolves from weak three-to two-dimensional character.These results are helpful to gain more insight into the nature of high-temperature superconductivity with dimensionality.

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.

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.

Effect of drying methods on perovskite films and solar cells

The high efficiency,solution processibility,and flexibility of perovskite solar cells make them promising candidates for the photovoltaic industry[1−8].The deposition method is one of the most critical factors that affect the performance of perovskite films.Various deposition methods have been developed to make perovskite films,including spin-coating,slotdie coating.

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.