Recently theorized hybrid II-IV-N{_2} / III-N heterostructures, based on current commercialized (In,Ga)N devices, are predicted to significantly advance the design space of highly efficient optoelectronics in the visible spectrum, yet there are few epitaxial studies of II-IV-N{_2} materials. In this work, we present heteroepitaxial ZnGeN{_2} grown on GaN buffers and AlN templates. We demonstrate that a GaN nucleating surface is crucial for increasing the ZnGeN{_2} crystallization rate to combat Zn desorption, extending the stoichiometric growth window from 215 {\degree}C on AlN to 500 {\degree}C on GaN buffers. Structural characterization reveals well crystallized films with threading dislocations extending from the GaN buffer. These films have a critical thickness for relaxation of 20 nm - 25 nm as determined by reflection high energy electron diffraction (RHEED) and cross-sectional scanning electron microscopy (SEM). The films exhibit a cation-disordered wurtzite structure, with lattice constants a = 3.216 Å {\pm} 0.004 Å and c = 5.215 Å {\pm} 0.005 Å determined by RHEED and X-ray diffraction (XRD). This work demonstrates a significant step towards the development of hybrid ZnGeN{_2}-GaN integrated devices.
Epitaxial Mn-doped BiFeO3 (MBFO) thin films were grown on GaAs (001) substrate with SrTiO3 (STO) buffer layer by pulsed laser deposition. X-ray diffraction results demonstrate that the films show pure (00l) orientation, and MBFO(100)//STO(100), whereas STO (100)//GaAs (110). Piezoresponse force microscopy images and polarization versus electric field loops indicate that the MBFO films grown on GaAs have an effective ferroelectric switching. The MBFO films exhibit good ferroelectric behavior (2Pr ~ 92 μC/cm2 and 2EC ~ 372 kV/cm). Ferromagnetic property with saturated magnetization of 6.5 emu/cm…
Heteroepitaxial Growth of PbSe on InP Substrates via Lattice-Matched III-V Buffer Layers
CREOL, The College of Optics and Photonics, University of Central Florida（中佛罗里达大学光学与光子学院）；Department of Materials Science and Engineering, University of Central Florida（中佛罗里达大学材料科学与工程系）
Epitaxy of oxide materials on silicon (Si) substrates is of great interest for future functional devices using the large variety of physical properties of the oxides as ferroelectricity, ferromagnetism, or superconductivity. Recently, materials with high spin polarization of the charge carriers have become interesting for semiconductor-oxide hybrid devices in spin electronics. Here, we report on pulsed laser deposition of magnetite (Fe3O4) on Si(001) substrates cleaned by an in situ laser beam high temperature treatment. After depositing a double buffer layer of titanium nitride (TiN) and magn…
The heteroepitaxial growth of Re (0001) films on Nb (110) surfaces has been investigated. Nb/Re bilayers were grown on A-plane sapphire -- alpha-Al2O3 (11-20) -- by molecular beam epitaxy. While Re grew with a (0001) surface, the in-plane epitaxial relationship with the underlying Nb could be best described as a combination of Kurdjumov-Sachs and Nishiyama-Wassermann orientations. This relationship was true regardless of Re film thickness. However, an evolution of the surface morphology with increasing Re thickness was observed, indicative of a Stranski-Krastanov growth mode. Re (0001) layers …
We report the successful growth of high-quality SrO films on highly-ordered pyrolytic graphite (HOPG) and single-layer graphene by molecular beam epitaxy. The SrO layers have (001) orientation as confirmed by x-ray diffraction (XRD) while atomic force microscopy measurements show continuous pinhole-free films having rms surface roughness of <1.5 Å. Transport measurements of exfoliated graphene after SrO deposition show a strong dependence between the Dirac point and Sr oxidation. Subsequently, the SrO is leveraged as a buffer layer for more complex oxide integration via the demonstration of (0…
A free-standing bulk gallium nitride layer with a thickness of 365 $μ$m and a diameter of 50 mm was obtained by hydride vapor phase epitaxy on a sapphire substrate with a carbon buffer layer. The carbon buffer layer was deposited by thermal decomposition of methane $\textit{in situ}$ in the same process with the growth of a bulk GaN layer. The bulk GaN layer grown on the carbon buffer layer self-separated from the sapphire substrate during the cooling after the growth. The dislocation density was $8\cdot10^{6}$ cm$^{-2}$. The (0002) X-Ray rocking curve full width at half maximum was 164 arcsec…
Zinc-based nitride CaZn2N2 films grown by molecular beam epitaxy (MBE) with a plasma-assisted active nitrogen-radical source are promising candidates of next-generation semiconductors for light-emitting diodes and solar cells. This nitride compound has previously only been synthesized in a bulk form by ultrahigh-pressure synthesis at 5 GPa. Three key factors have been found to enable heteroepitaxial film growth: (i) precise tuning of the individual flux rates of Ca and Zn, (ii) the use of GaN template layers on sapphire c-plane as substrates, and (iii) the application of MBE with an active N-r…
Interfacial Coupling Controls Molecular Epitaxy of HMTP on Graphene/SiC
Masaryk University（马萨里克大学）；Brno University of Technology（布尔诺理工大学）；Charles University（查理大学）；Institute of Physical Engineering, Brno University of Technology（布尔诺理工大学物理工程学院）
Transition metal oxides show fascinating physical properties such as high temperature superconductivity, ferro- and antiferromagnetism, ferroelectricity or even multiferroicity. The enormous progress in oxide thin film technology allows us to integrate these materials with semiconducting, normal conducting, dielectric or non-linear optical oxides in complex oxide heterostructures, providing the basis for novel multi-functional materials and various device applications. Here, we report on the combination of ferromagnetic, semiconducting, metallic, and dielectric materials properties in thin fil…
Controlled epitaxy of room-temperature quantum emitters in gallium nitride
School of Engineering, Cardiff University（卡迪夫大学工程学院）；Translational Research Hub（转化研究枢纽）；Department of Materials Science and Metallurgy, University of Cambridge（剑桥大学材料科学与工程系）
We report on the growth of epitaxial ZnO thin films and ZnO based heterostructures on sapphire substrates by laser molecular beam epitaxy (MBE). We first discuss some recent developments in laser-MBE such as flexible ultra-violet laser beam optics, infrared laser heating systems or the use of atomic oxygen and nitrogen sources, and describe the technical realization of our advanced laser-MBE system. Then we describe the optimization of the deposition parameters for ZnO films such as laser fluence and substrate temperature and the use of buffer layers. The detailed structural characterization b…
Reflection high-energy electron diffraction (RHEED) is a ubiquitous in situ molecular beam epitaxial (MBE) characterization tool. Although RHEED can be a powerful means for crystal surface structure determination, it is often used as a static qualitative surface characterization method at discrete intervals during a growth. A full analysis of RHEED data collected during the entirety of MBE growths is made possible using principle component analysis (PCA) and k-means clustering to examine significant boundaries that occur in the temporal clusters grouped from RHEED data and identify statistical…
We investigate the complex relationship between the growth conditions and the structural and transport properties of $\mathrm{Ti_xO_y}$ thin films grown by molecular beam epitaxy. Transport properties ranging from metallicity to superconductivity and insulating states are stabilized by effectively tuning the O/Ti ratio via the Ti flux rate and the O partial pressure, $P_{Ox}$, for films grown on (0001)-$\mathrm{Al_2 O_3}$ substrates at 850$^{\circ}$ C. A cubic $c-\mathrm{TiO_{1\pmδ}}$ buffer layer is formed for low O/Ti ratios while a corundum cr-$\mathrm{Ti_2 O_3}$ layer is formed under highe…
La2/3Ca1/3MnO3 thin films have been grown on yttria-stabilized zirconia (YSZ) buffered silicon-on-insulator (SOI) substrate by the pulsed laser deposition technique. While full cube-on-cube epitaxy was achieved for the YSZ layer, the top manganite layer was multi-domain-oriented, with a coexistence of cube-on-cube and cube-on-diagonal epitaxy. Due to a combined influence from the magnetocrystalline anisotropy and the magnetoelastic anisotropy, in zero field the local spin orientation varies across the twin boundaries. As a result, a quite large low-field magnetoresistance (LFMR) based on spin-…
Epitaxial thin films of the highly spin polarized Heusler compound Co2Cr0.6Fe0.4Al are deposited by dc magnetron sputtering. It is shown by XRD and TEM investigations how the use of an Fe buffer layer on MgO(100) substrates supports the growth of highly ordered Co2Cr0.6Fe0.4Al at low deposition temperatures. The as grown samples show a relatively large ordered magnetic moment of mu = 3.0mu_B/f.u. providing evidence for a low level of disorder.
Molecular beam epitaxy offers an exciting avenue for investigating the behavior of topological semimetal Cd3As2, by providing routes for doping, alloying, strain engineering, and heterostructure formation. To date, however, minimal exploration has been devoted to the impact of defects that are incorporated into epilayers due to contraints imposed by the substrate and narrow growth window. Here, we use a combination of lattice-matched ZnxCd1-xTe buffer layers, miscut substrates and broadband illumination to study how dislocations, twins and point defects influence the electron mobility of Cd3As…
We demonstrate the making of BaZrS3 thin films by molecular beam epitaxy (MBE). BaZrS3 forms in the orthorhombic distorted-perovskite structure with corner-sharing ZrS6 octahedra. The single-step MBE process results in films smooth on the atomic scale, with near-perfect BaZrS3 stoichiometry and an atomically-sharp interface with the LaAlO3 substrate. The films grow epitaxially via two, competing growth modes: buffered epitaxy, with a self-assembled interface layer that relieves the epitaxial strain, and direct epitaxy, with rotated-cube-on-cube growth that accommodates the large lattice consta…
Strain-released epitaxy of GaN enabled by compliant single-crystalline metal foils
Zhejiang University（浙江大学）；Westlake University（西湖大学）；Zhongke Crystal Materials (Dongguan) Technology Co., Ltd.（中科晶材（东莞）科技有限公司）；Institute of Semiconductors, Chinese Academy of Sciences（中国科学院半导体研究所）；Westlake Smoky-mountain Technologies（西湖烟山科技有限公司）；Peking University（北京大学）；University of Toronto（多伦多大学）；BOE Technology Group Co., Ltd.（京东方科技集团股份有限公司）
High-index Bi2Se3(221) film has been grown on In2Se3-buffered GaAs(001), in which a much retarded strain relaxation dynamics is recorded. The slow strain-relaxation process of in epitaxial Bi2Se3(221) can be attributed to the layered structure of Bi2Se3 crystal, where the epifilm grown along [221] is like a pile of weakly-coupled quintuple layer slabs stacked side-by-side on substrate. Finally, we have revealed the strong chemical bonding at the interface of Bi2Se3 and In2Se3 by plotting differential charge contour calculated by first-principle method. This study points to the feasibility of a…
Raman spectroscopy is utilized to study the magnetic characteristics of heteroepitaxial NiO thin films grown by plasma-assisted molecular beam epitaxy on MgO(100) substrates. For the determination of the Néel temperature, we demonstrate a reliable approach by analyzing the temperature dependence of the Raman peak originating from second-order scattering by magnons. The antiferromagnetic coupling strength is found to be strongly influenced by the growth conditions. The low-temperature magnon frequency and the Néel temperature are demonstrated to depend on the biaxial lattice strain and the degr…
As-grown superconducting MgB_2 thin films have been grown on SrTiO_3(001), MgO(001), and Al_2O_3(0001) substrates by a molecular beam epitaxy (MBE) method with novel co-evaporation conditions of low deposition rate in ultra-high vacuum. The structural and physical properties of the films were studied by RHEED, XRD, electrical resistivity measurements, and SQUID magnetometer. The RHEED patterns indicate three-dimensional growth for MgB_2. The highest T_c determined by resistivity measurement was about 36K in these samples. And a clear Meissner effect below T_c was observed using magnetic suscep…
Here we report a method to fabricate high quality Bi2Se3 thin films using molecular beam epitaxy with a radio frequency cracker cell as an atomic selenium source. With rates close to exact stoichiometry, optimal layer-by-layer growth of high quality Bi2Se3 thin films with smooth surfaces, has been achieved on CaF2(111) substrates and Si(111) substrates with a thin CaF2 buffer layer(CaF2/Si). Transport measurements show a characteristic weak antilocalization mangnetoresistance, with emergence of weak localization in the ultrathin film limit. Quantum Oscillations attributed to the topological su…
Cubic (zinc-blende) Ga1-xMnxN layers were grown by plasma-assisted molecular beam epitaxy on GaAs (001) substrates. Some of the structures also contained cubic AlN buffer layers. Auger Electron Spectroscopy and Secondary Ion Mass Spectroscopy studies clearly confirmed the incorporation of Mn into cubic GaN, the Mn being uniformly distributed through the layer. X-ray diffraction studies demonstrated that the Mn-doped GaN films are cubic and do not show phase separation up to a Mn concentrations of x<0.1. P-type conductivity for the cubic Ga1-xMnxN layers was observed for a wide range of the Mn …
SrMoO$_3$ is a promising material for its excellent electrical conductivity, but growing high-quality thin films remains a challenge. Here we synthesized epitaxial films of SrMoO$_3$ using the molecular beam epitaxy (MBE) technique under a low oxygen-flow rate. Introduction of SrTiO$_3$ buffer layers of 4--8 unit cells between the film and the (001)-oriented SrTiO$_3$ or KTaO$_3$ substrate was crucial to remove impurities and/or roughness of the film surface. The obtained film shows improved electrical conductivities as compared with films obtained by other techniques. The high quality of the …
Several ten $μ$m GaN have been deposited on a silicon substrate using a two-step hydride vapor phase epitaxy (HVPE) process. The substrates have been covered by AlN layers and GaN nanostructures grown by plasma-assisted molecular-beam epitaxy. During the first low-temperature (low-T) HVPE step, stacking faults (SF) form, which show distinct luminescence lines and stripe-like features in cathodoluminescence images of the cross-section of the layers. These cathodoluminescence features allow for an insight into the growth process. During a second high-temperature (high-T) step, the SFs disappear,…
The structure of titanium films on α- Al2O3(0001) surfaces at room temperature was investigated through in situ reflection high energy electron diffraction (RHEED). The α-phase of titanium was observed to grow with the Ti(0001) || Al2O3(0001), Ti[1100] || Al2O3[2110] and Ti[1010] || Al2O3[1100] epitaxy. For up to 6 nm thick films, an other structure was found to coexist with α-Ti. Its presence has dramatic consequences for the wetting of silver, which partly explains the nontrivial buffer effect of titanium at the silver/alumina interface. From the RHEED data, the extra structure is assigned t…
We demonstrate a new substrate cleaning and buffer growth scheme in $β$-Ga$_2$O$_3$ epitaxial thin films using metalorganic vapor phase epitaxy (MOVPE). For the channel structure, a low-temperature (LT, 600 $^\circ$C) undoped Ga$_2$O$_3$ buffer is grown followed by transition layers to a high-temperature (HT, 810 $^\circ$C) Si-doped Ga$_2$O$_3$ channel layers without growth interruption. The (010) Ga$_2$O$_3$ Fe-doped substrate cleaning uses solvent cleaning followed by an additional HF (49% in water) treatment for 30 mins before the epilayer growth. This step is shown to compensate the parasi…
The naturally existing chalcogenide Bi2Se3 is topologically nontrivial due to the band inversion caused by strong spin-orbit coupling inside the bulk of the material. The surface states are spin polarized, protected by the time-inversion symmetry, and thus robust to the scattering caused by non-magnetic defects. A high purity topological insulator thin film can be easily grown via molecular beam epitaxy (MBE) on various substrates to enable novel electronics, optics, and spintronics applications. However, the unique surface state properties have historically been limited by the film quality, w…
The superconductor Sn$_{1-x}$In$_{x}$Te is derived from the topological crystalline insulator SnTe and is a candidate topological superconductor. So far, high-quality thin films of this material have not been available, even though such samples would be useful for addressing the nature of its superconductivity. Here we report the successful molecular beam epitaxy growth of superconducting Sn$_{1-x}$In$_{x}$Te films by using Bi$_2$Te$_3$ as a buffer layer. The data obtained from tunnel junctions made on such films show the appearance of two superconducting gaps, which points to the coexistence …
Growth optimization of shallow Ge quantum wells grown by molecular beam epitaxy
Laboratory for Physical Sciences（物理科学实验室）；Department of Physics, University of Maryland（马里兰大学物理系）；Department of Materials Science & Engineering, University of Maryland（马里兰大学材料科学与工程系）
AlN layers with thicknesses between 2 and 14 nm were grown on Si(111) substrates by molecular beam epitaxy. The effect of the AlN layer thickness on the morphology and nucleation time of spontaneously formed GaN nanowires (NWs) was investigated by scanning electron microscopy and line-of-sight quadrupole mass spectrometry, respectively. We observed that the alignment of the NWs grown on these layers improves with increasing layer thickness while their nucleation time decreases. Our results show that 4 nm is the smallest thickness of the AlN layer that allows the growth of well-aligned NWs with…
Molecular beam epitaxy of single-crystalline bixbyite (In$_{1-x}$Ga$_x$)$_2$O$_3$ films ($x \leq 0.18$): Structural properties and consequences of compositional inhomogeneity
本文利用等离子体辅助分子束外延在 YSZ 衬底上生长单晶 (In$_{1-x}$Ga$_x$)$_2$O$_3$ 薄膜，发现 In$_2$O$_3$ 缓冲层可改善结晶质量，并揭示高 Ga 含量下 Ga 分布不均匀导致光谱性质饱和的现象。
The integration of MOCVD grown group III-A nitride device stacks on Si (111) substrates is critically dependent on the quality of the first AlN buffer layer grown. A Si surface that is both oxide-free and smooth is a primary requirement for nucleating such layers. A single parameter, the AlN layer growth stress, is shown to be an early (within 50 nm), clear (<0.5 GPa versus >1 GPa) and fail-safe indicator of the pre-growth surface, and the AlN quality required for successful epitaxy. Grain coalescence model for stress generation is used to correlate growth stress, the AlN-Si interface and crys…
Band structure engineering and interfacial buffer layers have been demonstrated as effective means to tune the Fermi level in topological insulators (TI). In particular, the charge compensated compound (BixSb1-x)2Te3 (BST) plays a critical role in the molecular beam epitaxy growth of magnetic TIs. Here we introduce a strategy of exploiting epitaxial Cr2O3 as a buffer layer and amorphous Cr2O3 as a capping layer in the growth of BST films. These films exhibit carrier density lower than 1012/cm2 over a wide range of Bi contents and higher mobility than BST films directly grown on Al2O3 substrate…
