Initial epitaxial growth of (111) Au/(111) Cu and (111) Cu/(111) Au

The room temperature modes of growth of Au/(111) Cu and Cu/(111) Au are described. For the former growth mode initial deposits (2.4 Å) of gold on copper form smooth flat islands delineated by coincidence lattice misfit dislocations. For 6.0 Å of gold deposit, both thick and thin gold areas were observed with almost complete substrate coverage. For a 10 Å deposit, surface coverage was complete. Strain measurements and dislocation densities obtained on the (111) Au/(111) Cu films suggest the presence of two separate misfit dislocation networks at the interface. The coincidence lattice networks were large enough for transmission electron microscopy observation but contributed little to total overlayer strain. The (van der Merwe) natural lattice misfit dislocations were too closely spaced for direct observation but their presence was inferred because of the strain measurements. The initial epitaxy of Cu/(111) Au was similar to the Stranski-Krastanov model: the initial monolayer of copper (also delineated by coincidence misfit dislocations) grew smoothly on the gold; additional copper formed essentially stress-free “nuclei” on top of the initial copper layer.     

Structural and optical properties of high quality ZnO thin film on Si with SiC buffer layer

ZnO thin films are grown on Si substrates with SiC buffer layer using ion plasma high frequency magnetron sputtering. These substrates are fabricated using a technique of solid phase epitaxy. With this technique SiC layer of thickness 20-200 nm had been grown on Si substrates consisting pores of sizes 0.5-5 μm at SiC and Si interface. Due to mismatching in lattice constants as well as thermal expansion coefficients, elastic stresses have been developed in ZnO film. Pores at the interface of SiC and Si are acting as the elastic stress reliever of the ZnO films making them strain free epitaxial. ZnO film grown on this especially fabricated Si substrate with SiC buffer layer exhibits excellent crystalline quality as characterized using X-ray diffraction. Surface topography of the film has been characterized using Atomic Force Microscopy as well as Scanning Electron Microscopy. Chemical compositions of the films have been analyzed using Energy Dispersive X-ray Spectroscopy. Optical properties of the films are investigated using Photoluminescence Spectroscopy which also shows good optical quality.     

Modulating Epitaxial Atomic Structure of Antimonene through Interface Design

Antimonene, a new semiconductor with fundamental bandgap and desirable stability, has been experimentally realized recently. However, epitaxial growth of wafer‐scale single‐crystalline monolayer antimonene preserving its buckled configuration remains a daunting challenge. Here, Cu(111) and Cu(110) are chosen as the substrates to fabricate high‐quality, single‐crystalline antimonene via molecular beam epitaxy (MBE). Surface alloys form spontaneously after the deposition and postannealing of Sb on two substrates that show threefold and twofold symmetry with different lattice constants. Increasing the coverage leads to the epitaxial growth of two atomic types of antimonene, both exhibiting a hexagonal lattice but with significant difference in lattice constants, which are observed by scanning tunneling microscopy. Scanning tunneling spectroscopy measurements reveal the strain‐induced tunable bandgap, in agreement with the first‐principles calculations. The results show that epitaxial growth of antimonene on different substrates allow the electronic properties of these films to be tuned by substrate‐induced strain and stress.     

Graphene–Mesoporous Si Nanocomposite as a Compliant Substrate for Heteroepitaxy

The ultimate performance of a solid state device is limited by the restricted number of crystalline substrates that are available for epitaxial growth. As a result, only a small fraction of semiconductors are usable. This study describes a novel concept for a tunable compliant substrate for epitaxy, based on a graphene–porous silicon nanocomposite, which extends the range of available lattice constants for epitaxial semiconductor alloys. The presence of graphene and its effect on the strain of the porous layer lattice parameter are discussed in detail and new remarkable properties are demonstrated. These include thermal stability up to 900 °C, lattice tuning up to 0.9 % mismatch, and compliance under stress for virtual substrate thicknesses of several micrometers. A theoretical model is proposed to define the compliant substrate design rules. These advances lay the foundation for the fabrication of a compliant substrate that could unlock the lattice constant restrictions for defect‐free new epitaxial semiconductor alloys and devices.     

ZnO薄膜的同质外延生长及其结构表征

利用等离子体辅助分子束外延的方法在ZnO单晶衬底上制备了ZnO薄膜。利用X射线衍射(XRD)、同步辐射掠入射XRD和φ扫描等实验技术研究了ZnO薄膜的结构。XRD和φ扫描的结果显示同质外延的ZnO薄膜已经达到单晶水平。掠入射XRD结果表明ZnO薄膜内部不同深度处a方向的晶格弛豫是不一致的,从接近衬底界面处到薄膜的中间部分再到薄膜的表面处,a方向的晶格常数分别为0.3249,0.3258和0.3242 nm。计算得到ZnO薄膜的泊松比为0.156,同质外延的ZnO薄膜与衬底在a轴方向的晶格失配度为-0.123%。     

X-ray absorption and Raman study of GaN films grown on different substrates by different techniques

Raman scattering and polarization-dependent synchrotron radiation X-ray absorption, in combination, have been employed to examine the residual stress of undoped GaN epitaxial layers grown on Si by molecular beam epitaxy and Si-doped n-type GaN layers grown on sapphire by metalorganic chemical vapor deposition. Values of the lattice constant of different GaN films can be deduced from the interatomic distances in the second coordination shell around Ga by polarization-dependent extended X-ray absorption fine structure analysis and the strain of the films can be obtained. This result is further confirmed by Raman scattering spectra in which the phonon modes show a significant shift between different GaN epitaxial layers with different growth conditions.     

Study of InN/GaN interfaces using molecular dynamics

Epitaxial growth of thin films is, in general, based on specific interfacial structures defined by a minimum of interfacial energy and usually influenced by the structural mismatch. In the present study, the structures and energies of (0001) InN/GaN epitaxial interfaces are studied using the Tersoff interatomic potential. The potential describes the metallic and intermetallic interactions sufficiently well and is assembled in order to accurately reproduce the lattice and elastic parameters of wurtzite Ga(In)-Nitrides. Different configurations are examined for each interface depending on polarity and atomic stacking. It is shown that the interfacial structures of InN thin films grown with indium polarity interfaces exhibit lower self-energies than those of N-polarity. Although the substrate and the epilayer were assumed to exhibit the wurtzite crystal structure, both wurtzite and zinc-blende type atomic stackings are possible at the interfacial region since they were found energetically degenerate within the accuracy of our model. Finally, the spatial location of the epitaxial interface is also energetically defined. Epitaxial interfaces in this system can in principle be imagined to pass through so-called single or double atomic bonds, but the former case was energetically more favourable.     

Brillouin scattering by surface acoustic modes for elastic characterization of ZnO films

Brillouin scattering from surface phonons was used for determining the dispersion curves of guided acoustic modes propagating along piezoelectric ZnO films. Measurements were performed on films of different thicknesses in the range between 20 and 320 nm, deposited by RF magnetron sputtering on Si and SiO(2) substrates. Brillouin spectra from Rayleigh acoustic modes are taken in the backscattering geometry at different incidence angles between 30 degrees and 70 degrees . The experimental data for the ZnO/Si films fit the expected theoretical dispersion curves fairly well for film thicknesses greater than 150 nm, while they appreciably depart from the same curves for smaller thicknesses. This behavior is interpreted in terms of a reduction of the effective elastic constants of the film in a layer near the interface, due to the lattice misfit between the film and the substrate. This effect was not observed in the case of ZnO films deposited on fused quartz substrates.     

Epitaxial Strain and Formation of the Interface Alloys in Layered System Fe/Cr

Ferromagnetic resonance (FMR) comparative measurements have been used to study the magnetic properties of rf sputtered ultra-thin single Fe-layer and Fe/Cr/Fe-trilayers on MgO(001) substrate. We state that in case of realization of a layer-by-layer epitaxial mode on the interface the ordered alloy is formatted. In case of a deviation from this mode, the critical layer, in which relaxes epitaxial strain induced by the lattice misfit between the overlayer and the substrate, is involved in formation of a disordered surface alloy. Difference of character of the epitaxial strain relaxation for the different misfit signature explains the difference of interfaces Cr/Fe and Fe/Cr.     

Investigation of the growth of In2O3 on Y-stabilized ZrO2(100) by oxygen plasma assisted molecular beam epitaxy

Thin films of In₂O₃ have been grown on Y-stabilised ZrO₂(100) substrates by oxygen plasma assisted molecular beam epitaxy over a range of substrate temperatures between 650 °C and 900 °C. Growth at 650 °C leads to continuous but granular films and complete extinction of substrate core level structure in X-ray photoelectron spectroscopy. However with increasing substrate temperature the films break up into a series of discrete micrometer sized islands. Both the continuous and the island films have excellent epitaxial relationship with the substrate as gauged by X-ray diffraction and selected area electron diffraction and lattice imaging in high resolution transmission electron microscopy.     

Bandgap modifications by lattice deformations in β-FeSi2 epitaxial films

The modifications of direct transition energies by lattice deformations were investigated in β-FeSi₂ epitaxial films, polycrystal films and single crystal, systematically. The lattice deformations depending on thermal annealing temperature (T_a) were observed in β-FeSi₂ epitaxial films. In photoreflectance (PR) measurements, the direct transition energies of the epitaxial films shifted to lower energies as the T_a increased. The polycrystal films did not show the lattice deformation and the shift of direct transition energies. These results show that the direct bandgap is modified by the lattice deformation originating from the lattice mismatch at the hetero-interface of β-FeSi₂/Si.     

Epitaxial growth of topological insulator Bi2Se3 film on Si(111) with atomically sharp interface

Atomically sharp epitaxial growth of Bi₂Se₃ films is achieved on Si(111) substrate with molecular beam epitaxy. Two-step growth process is found to be a key to achieve interfacial-layer-free epitaxial Bi₂Se₃ films on Si substrates. With a single-step high temperature growth, second phase clusters are formed at an early stage. On the other hand, with low temperature growth, the film tends to be disordered even in the absence of a second phase. With a low temperature initial growth followed by a high temperature growth, second-phase-free atomically sharp interface is obtained between Bi₂Se₃ and Si substrate, as verified by reflection high energy electron diffraction (RHEED), transmission electron microscopy (TEM) and X-ray diffraction. The lattice constant of Bi₂Se₃ is observed to relax to its bulk value during the first quintuple layer according to RHEED analysis, implying the absence of strain from the substrate. TEM shows a fully epitaxial structure of Bi₂Se₃ film down to the first quintuple layer without any second phase or an amorphous layer.     

Ultrahigh‐Detectivity Photodetectors with Van der Waals Epitaxial CdTe Single‐Crystalline Films

Van der Waals epitaxy (vdWE) is crucial for heteroepitaxy of covalence‐bonded semiconductors on 2D layered materials because it is not subject to strict substrate requirements and the epitaxial materials can be transferred onto various substrates. However, planar film growth in covalence‐bonded semiconductors remains a critical challenge of vdWE because of the extremely low surface energy of 2D materials. In this study, direct growth of wafer‐scale single‐crystalline cadmium telluride (CdTe) films is achieved on 2D layered transparent mica through molecular beam epitaxy. The vdWE CdTe films exhibit a flat surface resulting from the 2D growth regime, and high crystal quality as evidenced by a low full width at half maximum of 0.05° for 120 nm thick films. A perfect lattice fringe appears at the interfaces, implying a fully relaxed state of the epitaxial CdTe films correlated closely to the unique nature of vdWE. Moreover, the vdWE CdTe photodetectors demonstrate not only ultrasensitive optoelectronic response with optimal responsivity of 834 A W^?1 and ultrahigh detectivity of 2.4 × 10¹⁴ Jones but also excellent mechanical flexibility and durability, indicating great potential in flexible and wearable devices.     

Epitaxial growth of CoFe2O4 on SrTiO3 (100) and MgO (100) substrates without buffer layer by laser molecular beam epitaxy technique

Among the family of ferrite materials, cobalt ferrite (CoFe₂O₄) is unique in that it has the highest values of magneto-crystalline anisotropy and magnetostriction. Recently, much of the efforts have been focused on the fabrication of single crystalline cobalt ferrite films. For the epitaxial growth of cobalt ferrite, the issues of lattice parameter and crystal symmetry mismatch with the substrate are of considerable importance. The growth of thin films of CoFe₂O₄ on MgO and SrTiO₃ single crystal substrates is reported in this paper. The key parameters on the growth modes were investigated by changing oxygen pressure and substrate temperature. Results show that the two-dimensional layer-by-layer growth mode only occurs under high oxygen pressure for epitaxy of Co ferrite. The significant observation presents the controllable lattice constant of a highly strained thin film by modulation of the substrate temperature. In this light, to grow high quality Co ferrite thin films on SrTiO₃ is of a considerable importance to modulate intrinsic magnetic properties.     

SiC/Al2O3界面结构的同步辐射X射线掠入射衍射研究

采用固源分子束外延技术,以Al2O3为衬底,在1100℃下制备SiC薄膜。利用同步辐射X射线掠入射(GID)实验技术对生长的样品的界面结构进行了研究。结果表明,薄膜面内存在压应变,同时发现薄膜晶体质量在远离薄膜和衬底界面区会逐渐变好。GID和X射线衍射的摇摆曲线结果表明薄膜中镶嵌块的扭转大于倾斜,说明SiC薄膜在垂直方向的晶格排列要比面内更加有序。     

Epitaxial growth of solution grown polyvinylchloride (PVC) films

Thin films of polyvinylchloride (PVC) have been grown epitaxially from three different solvents onto the (001) plane of rocksalt crystals by the isothermal immersion technique. The ranges of values of the growth parameters (temperature and concentration of the solution and immersion time) over which epitaxial growth is obtained have been established in each case. Films grown from a benzene and acetone mixture show epitaxy only at temperatures of 58°C or more and with concentrations below 0.1 g/100 ml. The epitaxial relation is (010) [110]_PVC∥(001) [110]_NaCl. The crystallites in the epitaxial films are of pyramidal shape and the molecular chains are folded in a direction perpendicular to the substrate. Films grown from ethyl methyl ketone solution show epitaxy only at temperatures of 65°C or more for concentrations greater than or equal to 0.15 g/100 ml. Films grown from cyclohexanone solution show epitaxy over a wide range of temperatures and concentrations. The epitaxial relation is (001) [110]_PVC∥(001) [110]_NaCl and the crystallites are rod- or fibre-like. The molecular chains in these crystallites are folded in a direction parallel to the substrate. Our studies show that epitaxial growth occurs in the earliest stage of growth of the films and further growth results in a mixture of amorphous and polycrystalline regions. The mechanism of epitaxial growth is explained in terms of our model for the growth of polymer chains. Two possible configurations of the molecular chains in the unit cell of PVC on a (001) rocksalt surface are proposed to explain the two epitaxial orientation relations observed.     

Epitaxial growth of nanostructured gold films on germanium via galvanic displacement

This work focuses on the synthesis and characterization of gold films grown via galvanic displacement on Ge(111) substrates. The synthetic approach uses galvanic displacement, a type of electroless deposition that takes place in an efficient manner under aqueous, room temperature conditions. Investigations involving X-ray diffraction (XRD) and transmission electron microscopy (TEM) techniques were performed to study the crystallinity and orientation of the resulting gold-on-germanium films. A profound effect of HF(aq) concentration was noted, and although the SEM images did not show significant differences in the resulting gold films, a host of X-ray diffraction studies demonstrated that higher concentrations of HF(aq) led to epitaxial gold-on-germanium, whereas in the absence of HF(aq), lower degrees of order (fiber texture) resulted. Cross-sectional nanobeam diffraction analyses of the Au-Ge interface confirmed the epitaxial nature of the gold-on-germanium film. This epitaxial behavior can be attributed to the simultaneous etching of the germanium oxides, formed during the galvanic displacement process, in the presence of HF. High-resolution TEM analyses showed the coincident site lattice (CSL) interface of gold-on-germanium, which results in a small 3.8% lattice mismatch due to the coincidence of four gold lattices with three of germanium.     

Equilibrium surface roughness of a strained epitaxial film due to surface diffusion induced by interface misfit dislocations

In recent years, developments in the microelectronics industry have led to extensive studies of the growth and characterization of thin solid films and their implementation in electronic and opto-electronic devices. A goal is to produce thin films with minimal bulk and surface defects. For those systems produced by epitaxial growth of a film on a substrate that has a slightly different lattice parameter, the stress associated with the elastic mismatch strain needed to satisfy the constraint of epitaxy provides a driving force for nucleation and growth of undesirable defects in the film material or on its surface. Among the most common defects are interface misfit dislocations, arranged more or less periodically on the film-substrate interface, which partially relax the elastic mismatch strain in the film. It has been observed that, for some material systems, surface roughness or waviness arises which correlates spatially with the positions of interface misfit dislocations. It is suggested here that the waviness along the surface may be a result of surface diffusion which is driven by a gradient in the chemical potential of the material along the surface. The chemical potential gradient arises from the nonuniform strain field of the interface misfit dislocations, as well as from the unrelaxed elastic mismatch strain. The focus here is on the development of a relatively simple model of this system which leads to an estimate of the magnitude and profile of surface waviness under conditions of thermodynamic equilibrium, i.e., after the material responds to the chemical potential gradient by seeking out a new configuration for which stresses are redistributed and the chemical potential is again uniform. The condition of uniform chemical potential for the final shape leads to an integro-differential equation for the equilibrium surface shape which is solved numerically. For representative values of system parameters, estimates of equilibrium surface roughness are obtained which can vary from less than one percent of film thickness to a significant fraction of film thickness. Although transient aspects of the process are not studied here, the characteristic time for achieving an equilibrium configuration is estimated.     

Delamination of thin film strips

Delamination of residually stressed thin film strips is analyzed to expose the dependence on strip width and film/substrate elastic mismatch. Isotropic films and substrates are assumed. The residual stress in the film is tensile and assumed to originate from mismatch due to thermal expansion or epitaxial deposition. Full and partial delamination modes are explored. In full delamination, the interface crack extends across the entire width of the strip and releases all the elastic energy stored in the strip as the crack propagates along the interface. The energy release rate available to propagate the interface crack is a strong function of the strip width and the elastic modulus of the film relative to that of the substrate. The energy release rate associated with full delamination is determined as a function of the interface crack length from initiation to steady-state, revealing a progression of behavior depending in an essential way on the three dimensionality of the strip. The dependence of the energy release rate on the remaining ligament as the interface crack converges with the strip end has also been calculated, and the results provide an effective means for inferring interface toughness from crack arrest position. A partial delamination propagates along the strip leaving a narrow width of strip attached to the substrate. In this case, the entire elastic energy stored in the strip is not released because the strain component parallel to the strip is not relaxed. A special application is also considered, in which a residually stressed metal superlayer is deposited onto a polymer strip. The energy release rate for an interface crack propagating along the interface between the polymer and the substrate is determined in closed form.