Molecular dynamics study of interfaces in solids

The interfaces of heterostructures were studied in the framework of molecular dynamics to reveal a periodic interface stress distribution on the micro scale. The calculations were performed for copper and silver and for two different types of heterostructures: a heterostructure consisting of perfect Cu and Ag crystals and a heterostructure formed by Ag vapor deposition on a perfect Cu substrate. The calculation results allowed several conclusions about the origin of a chessboard interface structure and about certain mechanisms of its modification depending on the nanostructure size, boundary conditions, and method of heterostructure formation.     

石墨烯-六方氮化硼面内异质结构的扫描隧道显微学研究

石墨烯-六方氮化硼面内异质结构因可调控石墨烯的能带结构而受到广泛关注. 本文介绍了在超高真空体系内, 利用两步生长法在两类对石墨烯分别有强和弱电子掺杂的基底, 即Rh(111)和Ir(111)上制备石墨烯-六方氮化硼单原子层异质结构. 通过扫描隧道显微镜及扫描隧道谱对这两种材料的形貌和电子结构进行研究发现: 石墨烯和六方氮化硼倾向于拼接生长形成单层的异质结构, 而非形成各自分立的畴区; 在拼接边界处, 石墨烯和六方氮化硼原子结构连续无缺陷; 拼接边界多为锯齿形型, 该实验结果与密度泛函理论计算结果相符合; 拼接界面处的石墨烯和六方氮化硼分别具有各自本征的电子结构, 六方氮化硼对石墨烯未产生电子掺杂效应.     

The Atomic Structure of Oxide/Oxide Interface

The physical and chemical properties of thin or ultrathin oxide film deposited on another oxide bulk or thin film usually differ strongly from the bulk. The properties of the heterostructures ultimately rely on the structure and the chemistry of the oxide/oxide interface. Data in the literature indicated that atomically abrupt interfaces between oxides show abnormal electronic and magnetic properties. This article reviews the interfacial structures of oxide/oxide interfaces in an atomic scale. The origins of the unique physical and chemical properties at the oxide/oxide interfaces are also discussed.     

Perspectives of cross-sectional scanning tunneling microscopy and spectroscopy for complex oxide physics

Complex oxide heterostructure interfaces have shown novel physical phenomena which do not exist in bulk materials. These heterostructures can be used in the potential applications in the next generation devices and served as the playgrounds for the fundamental physics research. The direct measurements of the interfaces with excellent spatial resolution and physical property information is rather difficult to achieve with the existing tools. Recently developed cross-sectional scanning tunneling microscopy and spectroscopy (XSTM/S) for complex oxide interfaces have proven to be capable of providing local electronic density of states (LDOS) information at the interface with spatial resolution down to nanometer scale. In this perspective, we will briefly introduce the basic idea and some recent achievements in using XSTM/S to study complex oxide interfaces. We will also discuss the future of this technique and the field of the interfacial physics.     

Tamm interface states in ZnSe/BeTe periodic heterostructures

The spectral response of the lateral optical anisotropy of periodic undoped type-II ZnSe/BeTe heterostructures with nonequivalent interfaces was studied by ellipsometry. The spectra revealed two types of features corresponding to optical transitions with energies lying in the bandgap. The position of features of the first type does not depend on the heterostructure period. Features of the second type shift toward lower energies with decreasing period of the heterostructure. This behavior is explained in terms of a model taking into account the existence of electronic and hole interface states and of a mixed-type interface state.     

First principle study on interfacial interaction of black phosphorus and CsBr vdW heterostructure

Two dimensional crystalline materials have attracted much attentions due to the establishment of heterostructure that can adjust their electrical and optical properties, and have potential applications in lasers, light-emitting diodes, solar cells and high mobility transistors. And the interface engineering is an effective route to tune structural and electrical properties in semiconductor heterostructures. In this study, the electronic structure, charge transport and optical properties of monolayer caesium bromide and black phosphorus (CsBr/BP) heterostructure are calculated by the first principle based on density functional theory (DFT). It was found that the characteristics of electronic band structures of the monolayer CsBr and BP remain in the heterostructure, and the effective mass and carrier mobility are highly anisotropic. When the heterostructure is uniaxially stretched, the mobility of electron is greater than that of the hole, while the biaxial stretching is just the opposite, the mobility of hole is greater than that of the electron. In addition, compared with the CsBr monolayer, the light absorption of the heterostructure is significantly enhanced, especially in the infrared, indicating that the CsBr/BP heterostructure can be well applied to photovoltaic devices in the future.     

Interface of transition metal oxides at the atomic scale

Remarkable phenomena arise at well-defined heterostructures, composed of transition metal oxides, which is absent in the bulk counterpart, providing us a paradigm for exploring the various electron correlation effects. The functional properties of such heterostructures have attracted much attention in the microelectronic and renewable energy fields. Exotic and unexpected states of matter could arise from the reconstruction and coupling among lattice, charge, orbital and spin at the interfaces. Aberration-corrected scanning transmission electron microscopy (STEM) is a powerful tool to visualize the lattice structure and electronic structure at the atomic scale. In the present study some novel phenomena of oxide heterostructures at the atomic scale are summarized and pointed out from the perspective of electron microscopy.     

Low-energy electron-excited nanoluminescence studies of GaN and related materials

We have used low-energy electron-excited nanoluminescence (LEEN) spectroscopy combined with ultrahigh vacuum surface analysis techniques to obtain electronic bandgap, confined state and deep-level trap information from III nitride compound semiconductor surfaces and their buried interfaces on a nanometer scale. Localized states are evident at GaN/InGaN quantum wells, GaN ultrathin films, AlGaN/GaN pseudomorphic heterostructures, and GaN/Al₂O₃ interfaces that are sensitive to the chemical composition, bonding and atomic structure near interfaces, and in turn to the specifics of the epitaxial growth process. Identification of electrically active defects in these multilayer nanostructures provides information to optimize interface growth and control local electronic properties.     

Interfacial defect engineering and photocatalysis properties of hBN/MX2 (M = Mo,W, and X = S,Se heterostructures

Van der Waals (VDW) heterostructures have attracted significant research interest due to their tunable interfacial properties and potential applications in many areas such as electronics, optoelectronic, and heterocatalysis. In this work, the influences of interfacial defects on the electronic structures and photocatalytic properties of hBN/MX₂ (M = Mo, W, and X=S, Se) are studied using density functional theory calculations. The results reveal that the band alignment of hBN/MX₂ can be adjusted by introducing vacancies and atomic doping. The type-I band alignment of the host structure is maintained in the heterostructure with n-type doping in the hBN sublayer. Interestingly, the band alignment changed into the type-II heterostructrue due to V_B defect and p-type doping is introduced into the hBN sublayer. This can conduce to the separation of photo-generated electron-hole pairs at the interfaces, which is highly desired for heterostructure photocatalysis. In addition, two Z-type heterostructures including hBN(Be_B)/MoS₂, hBN(Be_B)/MoSe₂, and hBN(V_N)/MoSe₂ are achieved, showing the decreasing of band gap and ideal redox potential for water splitting. Our results reveal the possibility of engineering the interfacial and photocatalysis properties of hBN/MX₂ heterostructures via interfacial defects.     

Atomic scale properties of interior interfaces of semiconductor heterostructures as determined by quasi-digital highly selective etching and atomic force microscopy

We report on first experiments combining quasi-digital highly selective etching and atomic force microscopy (AFM) to examine the interior interfaces of semiconductor heterostructures. Lattice matched (GaIn)As/InP heterostructures grown by metalorganic vapour-phase epitaxy (MOVPE) are taken as a model system to check the capabilities of this new method. Standard selective etchants for different material systems have been optimized in selectivity and etch rate to achieve a quasi-digital etching behaviour. In this way, the real structure of interior interfaces can be determined by AFM. We find a significant difference between the surface of the heterostructure and the interior interfaces.     

两步化学气相沉积法制备In2Se3/MoSe2范德华尔斯异质结

Two-dimensional transition metal dichalcogenides heterostructures have stimulated wide interest not only for the fundamental research,but also for the application of next generation electronic and optoelectronic devices.Herein,we report a successful two-step chemical vapor deposition strategy to construct vertically stacked van der Waals epitaxial In₂Se₃/MoSe₂ heterostructures.Transmission electron microscopy characterization reveals clearly that the In₂Se₃ has well-aligned lattice orientation with the substrate of monolayer MoSe₂.Due to the interaction between the In₂Se₃ and MoSe₂ layers,the heterostructure shows the quenching and red-shift of photoluminescence.Moreover,the current rectification behavior and photovoltaic effect can be observed from the heterostructure,which is attributed to the unique band structure alignment of the heterostructure,and is further confirmed by Kevin probe force microscopy measurement.The synthesis approach via van der Waals epitaxy in this work can expand the way to fabricate a variety of two-dimensional heterostructures for potential applications in electronic and optoelectronic devices.     

金辅助催化方法制备GaAs和GaAs/InGaAs纳米线结构的形貌表征及生长机理研究

利用金（Au）辅助催化的方法,通过金属有机化学气相沉积技术制备了GaAs纳米线及GaAs/InGaAs纳米线异质结构.通过对扫描电子显微镜（SEM）测试结果分析,发现温度会改变纳米线的生长机理,进而影响形貌特征.在GaAs纳米线的基础上制备了高质量的纳米线轴、径向异质结构,并对生长机理进行分析.SEM测试显示,GaAs/InGaAs异质结构呈现明显的“柱状”形貌与衬底垂直,InGaAs与GaAs段之间的界面清晰可见.通过X射线能谱对异质结样品进行了线分析,结果表明在GaAs/InGaAs轴向纳米线异质结构样品中,未发现明显的径向生长.从生长机理出发分析了在GaAs/InGaAs径向纳米线结构制备过程中伴随有少许轴向生长的现象.     

Electronic and optical properties of 3N-doped graphdiyne/MoS2 heterostructures tuned by biaxial strain and external electric field

The construction of van der Waals (vdW) heterostructures by stacking different two-dimensional layered materials have been recognised as an effective strategy to obtain the desired properties. The 3N-doped graphdiyne (N-GY) has been successfully synthesized in the laboratory. It could be assembled into a supercapacitor and can be used for tensile energy storage. However, the flat band and wide forbidden bands could hinder its application of N-GY layer in optoelectronic and nanoelectronic devices. In order to extend the application of N-GY layer in electronic devices, MoS₂ was selected to construct an N-GY/MoS₂ heterostructure due to its good electronic and optical properties. The N-GY/MoS₂ heterostructure has an optical absorption range from the visible to ultraviolet with a absorption coefficient of 10⁵ cm^-1. The N-GY/MoS₂ heterostructure exhibits a type-Ⅱ band alignment allows the electron-hole to be located on N-GY and MoS₂ respectively, which can further reduce the electron-hole complexation to increase exciton lifetime. The power conversion efficiency of N-GY/MoS₂ heterostructure is up to 17.77%, indicating it is a promising candidate material for solar cells. In addition, the external electric field and biaxial strain could effectively tune the electronic structure. Our results provide a theoretical support for the design and application of N-GY/MoS₂ vdW heterostructures in semiconductor sensors and photovoltaic devices.     

钙钛矿CsPbX3(X=Cl,Br,I)与五环石墨烯范德瓦耳斯异质结的界面相互作用和光电性能的第一性原理研究

异质结工程是一种提高半导体材料光电性能的有效方法.本文构建了全无机钙钛矿CsPbX₃(X=Cl,Br,I)和二维五环石墨烯penta-graphene(PG)的新型范德瓦耳斯(vdW)异质结,利用第一性原理研究了CsPbX₃-PG异质结不同界面接触的稳定性,进而计算了稳定性较好的Pb-X接触界面异质结的电子结构和光电性能.研究结果表明,CsPbX₃-PG(X=Cl,Br,I)异质结具有II型能带排列特征,能级差距由Cl向I逐渐缩小,具有良好的光生载流子分离能力和电荷输运性质.此外,研究发现CsPbX₃-PG异质结能有效拓宽材料的光吸收谱范围,并能显著提高其光吸收能力,尤其是CsPbI₃具有最优的光吸收性能.经理论估算,CsPbX₃-PG的光电功率转换效率(PCE)可高达21%.这些结果表明,全无机金属卤化物钙钛矿CsPbX₃-PG异质结可以有效地提高半导体材料的光电性能,预期在光电转换器件中具有重要的应用潜力.     

Computational screening of vdWs heterostructures of BSe with MoSe2 and WSe2 as sustainable hydrogen production materials

Recently, fabricating type-II vertical van der Waals (vdWs) heterostructure is a promising material for hydrogen production. The absorption capability, charge density distributions, band alignments and electronic properties of the monolayers and heterostructures are systematically investigated using computational studies. Using ab initio molecular dynamics, binding energy and phonon calculations, the stability of the heterostructures are verified. Both heterostructures are type-II materials, which can increase the separation of charge carriers. Moreover, the charge density difference and the potential drop across the interface of MSe₂/BSe creates a high built-in electric field that can prevent the recombination of charge carriers. We found that the visible-light optical properties of both heterostructures are much enhanced with suitable bandgap energy for water splitting. The band alignment suggests that the heterostructures straddle water redox potentials in acid solutions (0 < pH < 7). Our study predicted that MSe₂/BSe vdW heterostructures have great potential for photocatalytic hydrogen production.     

二维材料的转移方法

二维材料及其异质结在电子学、光电子学等领域具有潜在应用,是延续摩尔定律的候选电子材料.二维材料的转移对于物性测量与器件构筑至关重要.本文综述了一些具有代表性的转移方法,详细介绍了各个方法的操作步骤,并基于转移后样品表面清洁程度、转移所需时间以及操作难易等方面对各个转移方法进行了对比归纳.经典干、湿法转移技术是进行物理堆叠制备原子级平整且界面清晰范德瓦耳斯异质结的常用手段,结合惰性气体保护或在真空条件下操作还可以避免转移过程中二维材料破损和界面吸附.高效、无损大面积转移方法为二维材料异质结构建和材料本征物理化学性质测量提供了强有力的技术保障.转移技术的优化将进一步扩展二维材料在高温超导、拓扑绝缘体、低能耗器件、自旋谷极化、转角电子学和忆阻器等领域的研究.     

Hard X-ray photoemission spectroscopy: Variable depth analysis of bulk,surface and interface electronic properties

The electronic properties of surfaces and buried interfaces can vary considerably in comparison to the bulk. In turn, analyzing bulk properties, without including those of the surface, is understandably challenging. Hard X-ray photoelectron spectroscopy (HAXPES) allows the well known ability of photoemission to interrogate the electronic structure of material systems with bulk volume sensitivity. This is achieved by tuning the kinetic energy range of the analyzed photoelectrons in the multi-keV regime. This unique ability to probe truly bulk properties strongly compliments normal photoemission, which generally probes surface electronic structure that is different than the bulk selected examples of HAXPES and possible implications towards the study of complex oxide-based interfaces and highly correlated systems are discussed.     

Directly Determining the Interface Structure and Band Offset of a Large-Lattice-Mismatched CdS/CdTe Heterostructure

The CdS/CdTe heterojunction plays an important role in determining the energy conversion efficiency of CdTe solar cells.However,the interface structure remains unknown,due to the large lattice mismatch between CdS and CdTe,posing great challenges to achieving an understanding of its interfacial effects.By combining a neuralnetwork-based machine-learning method and the stochastic surface walking-based global optimization method,we first train a neural network potential for CdSTe systems with demonstrated robustness and reliability.Based on the above potential,we then use simulated annealing to obtain the optimal structure of the CdS/CdTe interface.We find that the most stable structure has the features of both bulks and disorders.Using the obtained structure,we directly calculate the band offset between CdS and CdTe by aligning the core levels in the heterostructure with those in the bulks,using one-shot first-principles calculations.Our calculated band offset is 0.55 eV,in comparison with 0.70 eV,obtained using other indirect methods.The obtained interface structure should prove useful for further study of the properties of CdTe/CdS heterostructures.Our work also presents an example which is applicable to other complex interfaces.     

ZnSe/GaAs(100)界面电子结构的计算

利用形式散射理论的格林函数方法，采用紧束缚最近邻近似下的sp³s模型，计算了ZnSe/GaAs(100)两类界面(Se/Ga和As/Zn界面)的电子结构.分别给出了两类界面的界面带结构和波矢分辨的层态密度及其分波态密度.计算结构表明，在ZnSe/GaAs(100)两类界面的禁带隙中均无界面态，而在其价带区均存在三条束缚的界面带和四条半共振带；通过比较，分析了两类界面的界面态特征及其来源. 关键词：     

Tunable electronic properties of GaS-SnS2 heterostructure by strain and electric field

Vertically stacked heterostructures have received extensive attention because of their tunable electronic structures and outstanding optical properties. In this work, we study the structural, electronic, and optical properties of vertically stacked GaS-SnS₂ heterostructure under the frame of density functional theory. We find that the stacked GaS-SnS₂ heterostructure is a semiconductor with a suitable indirect band gap of 1.82 eV, exhibiting a type-II band alignment for easily separating the photo-generated carriers. The electronic properties of GaS-SnS₂ heterostructure can be effectively tuned by an external strain and electric field. The optical absorption of GaS-SnS₂ heterostructure is more enhanced than those of the GaS monolayer and SnS₂ monolayer in the visible light region. Our results suggest that the GaS-SnS₂ heterostructure is a promising candidate for the photocatalyst and photoelectronic devices in the visible light region.