Nitride films are promising for advanced optoelectronic and electronic device applications. However, some challenges continue to impede development of high aluminum-containing devices. The two major difficulties are growth of high crystalline quality films with aluminum-rich compositions, and efficiently doping such films p-type. These problems have severely limited use of aluminum-rich nitride films grown by molecular beam epitaxy. A way around these problems is through use of a liquid-metal-enabled approach to molecular beam epitaxy. Although the presence of a liquid metal layer at the growth front is reminiscent of conventional liquid phase epitaxy, this approach is different in its details. Conventional liquid epitaxy is a near-thermodynamic equilibrium process which liquid-metal assisted molecular beam epitaxy is not. Growth of aluminum-rich nitrides is primarily driven by the kinetics of the molecular vapor fluxes, and the surface diffusion of adatoms through a liquid metal layer before incorporation. This paper reports on growth of high crystalline quality and highly doped aluminum-containing nitride films. Measured optical and electrical characterization data show that the approach is viable for growth of atomically smooth aluminum-containing nitride heterostructures. Extremely high p-type doping of up to $6 \times 10$$^{17}$ cm$^{-3}$ and n-type doping of up to $1 \times 10$$^{20}$ cm$^{-3}$ in Al$_{0.7}$Ga$_{0.3}$N films was achieved. Use of these metal-rich conditions is expected to have a significant impact on high efficiency and high power optoelectronic and electronic devices that require both high crystalline quality and highly doped (Al,Ga)N films.
RF plasma assisted MBE growth of Scandium Nitride (ScN) thin films on GaN (0001)/SiC, AlN (0001)/Al2O3 and on 6H-SiC (0001) hexagonal substrates is found to lead to a face centered cubic (rock-salt) crystal structure with (111) out-of-plane orientation instead of hexagonal orientation. For the first time, cubic (111) twinned patterns in ScN are observed by in-situ electron diffraction during epitaxy, and the twin domains in ScN are detected by electron backscattered diffraction, and further corroborated with X-ray diffraction. The epitaxial ScN films display very smooth, sub nanometer surface …
Hexagonal boron nitride (hBN) has been grown on sapphire substrates by ultra-high temperature molecular beam epitaxy (MBE). A wide range of substrate temperatures and boron fluxes have been explored, revealing that high crystalline quality hBN layers are grown at high substrate temperatures, $>$1600$^\circ$C, and low boron fluxes, $\sim1\times10^{-8}$ Torr beam equivalent pressure. \emph{In-situ} reflection high energy electron diffraction (RHEED) revealed the growth of hBN layers with $60^\circ$ rotational symmetry and the $[11\bar20]$ axis of hBN parallel to the $[1\bar100]$ axis of the sapp…
We report a complementary metal oxide semiconductor (CMOS) technology compatible ferroelectric tunnel junction memristor grown directly on top of a Silicon substrate using a scandium doped aluminum nitride as the ferroelectric layer.
Aluminum nitride (AlN) is an emerging material for integrated quantum photonics with its excellent linear and nonlinear optical properties. In particular, its second-order nonlinear susceptibility $χ^{(2)}$ allows single-photon generation. We have grown AlN thin films on silicon nitride via reactive DC magnetron sputtering. The thin films have been characterized using X-ray diffraction, optical reflectometry, atomic force microscopy, and scanning electron microscopy. The crystalline properties of the thin films have been improved by optimizing the nitrogen to argon ratio and the magnetron DC p…
By using ab inito calculations within Density Functional Theory, we have explored the possible structures and various properties of porous AlN monolayer materials. Two kinds of porous AlN monolayer are identified, and the phonon dispersion spectrum together with the ab inito molecular dynamics simulations demonstrate that their structures are stable. We further show that these AlN porous monolayers have well-defined porous nanostructures and even higher specific surface areas, namely, which can be comparable with graphene, and can also be maintained evenly at high temperatures. Furthermore, bo…
Novel ohmic contacts to n-ZnSe are demonstrated using single crystal Al films deposited on epitaxially grown ZnSe (100) by molecular beam epitaxy (MBE). Electron Backscatter Diffraction (EBSD) confirmed the single crystalline structure of the Al films. The (110)-oriented Al layer was rotated rotated 45$^\circ$ relative to substrate to match the ZnSe (100) lattice constant. The as-grown Al-ZnSe contact exhibited nearly ideal ohmic characteristics over a large doping range of n-ZnSe without any additional treatment. The contact resistances are in a range of 10$^{-3}$ $Ω$-cm$^{2}$ for even lightl…
Systematic comparison of approximations and functionals in first-principle calculations of aluminum-based III-V ferroelectric nitrides
University of Arkansas（阿肯色大学）；Guangdong Technion – Israel Institute of Technology（广东以色列理工学院）；Colorado School of Mines（科罗拉多矿业学院）；National Laboratory of the Rockies（落基山国家实验室）；Tel Aviv University（特拉维夫大学）；Université Paris-Saclay（巴黎萨克雷大学）；CentraleSupélec（中央苏佩雷勒高等电信学院）
Machine learning is changing how we design and interpret experiments in materials science. In this work, we show how unsupervised learning, combined with ab initio modeling, improves our understanding of structural metastability in multicomponent alloys. We use the example case of Al-O-N alloys where the formation of aluminum vacancies in wurtzite AlN upon the incorporation of substitutional oxygen can be seen as a general mechanism of solids where crystal symmetry is reduced to stabilize defects. The ideal AlN wurtzite crystal structure occupation cannot be matched due to the presence of an a…
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）
Leibniz-Institut für Kristallzüchtung（莱布尼茨晶体生长研究所）
In this work, we study the absorption properties of AlN in the range of 1.5 - 5.5 eV, as well as the meta-stable change in absorption induced by ultraviolet (UV) irradiation (photochromism), and the restoration of the initial state under the action of irradiation of 2 - 4 eV or elevated temperatures. UV irradiation results in a decrease of the absorption coefficient from 110 cm$^{-1}$ to 55 cm$^{-1}$ at 4.7 eV while in the visible range the absorption coefficient increases from values below 5 cm$^{-1}$ to ~35 cm$^{-1}$. Measurements with two linear polarizations, parallel and perpendicular to …
Effect of the growth temperature and the AlN mole fraction on In incorporation and properties of quaternary III-nitride layers grown by molecular beam epitaxy
Acoustic and Optical Phonon Frequencies and Acoustic Phonon Velocities in Silicon-Doped Aluminum Nitride Thin Films
University of California, Los Angeles（加州大学洛杉矶分校）；California NanoSystems Institute, University of California, Los Angeles（加州大学洛杉矶分校加利福尼亚纳米系统研究所）；Arizona State University（亚利桑那州立大学）；Auburn University（奥本大学）
The control over the structural homogeneity is of paramount importance for ternary nitride compounds - the second most important semiconducting material-class after Si, due to its unrivalled applicability in optoelectronics, and high power/high frequency electronics. Therefore it is timely to investigate possible mechanisms influencing the crystallographic constitution of the material. In this work the diffusion mechanism of manganese in gallium nitride is investigated in two types of epilayers: Mn implanted metalorganic vapour phase epitaxy grown GaN and (Ga,Mn)N solid solution grown by molec…
Epitaxy of Fe3O4 on Si(001) by pulsed laser deposition using a TiN/MgO buffer layer
氧化物材料在硅（Si）衬底上的外延对于使用氧化物的各种物理性质如铁电性、铁磁性或超导性的未来功能器件具有极大的兴趣。最近，具有高自旋极化的载流子的材料已经成为自旋电子学中的氧化物-氧化物混合器件的关注点。在这里，我们报告的脉冲激光沉积磁铁矿（Fe 3 O 4）在Si（001）衬底上清洁的原位激光束高温处理。在沉积氮化钛（TiN）和氧化镁（MgO）的双缓冲层之后，可以生长高质量的外延磁铁矿层，如通过RHEED强度振荡和高分辨率X射线衍射所验证的。
Single layer hexagonal boron nitride is produced on 2 inch Pt(111)/sapphire wafers. The growth with borazine vapour deposition at process temperatures between 1000 and 1300 K is in-situ investigated by photoelectron yield measurements. The growth kinetics is slower at higher temperatures and follows a tanh$^2$ law which better fits for higher temperatures. The crystal-quality of h-BN/Pt(111) is inferred from scanning low energy electron diffraction (x-y LEED). The data indicate a strong dependence of the epitaxy on the growth temperature. The dominant structure is an aligned coincidence lattic…
The effect of film morphology on its surface chemistry and band structure has been analyzed for gallium nitride epitaxial films grown by molecular beam epitaxy. The film morphology has been studied using scanning electron microscopy and atomic force microscopy, and the bandstructure, defect and emission properties have been studied by X ray photoelectron spectroscopy and cathodoluminescence spectroscopy. It was found that the highly porous GaN nanowall network shows the highest relative conductivity and does not have defect related luminescence. The flatter films were more resistive and showed…
In 1963, Moll and Tarui suggested that the field-effect conductance of a semiconductor could be controlled by the remanent polarization of a ferroelectric (FE) material to create a ferroelectric field-effect transistor (FE-FET). However, subsequent efforts to produce a practical, compact FE-FET have been plagued by low retention and incompatibility with Complementary Metal Oxide Semiconductor (CMOS) process integration. These difficulties led to the development of trapped-charge based memory devices (also called floating gate or flash memory), and these are now the mainstream non-volatile memo…
$WSe_2$ Monolayers Grown by Molecular Beam Epitaxy on hBN
Institute of Experimental Physics, Faculty of Physics, University of Warsaw（华沙大学物理学院实验物理研究所）；Institute of Physics, Polish Academy of Sciences（波兰科学院物理研究所）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（国家材料科学研究所材料纳米构造研究中心）；Research Center for Electronic and Optical Materials, National Institute for Materials Science（国家材料科学研究所电子与光学材料研究中心）
The combination of two-dimensional (2D) materials into heterostructures enabled the formation of atomically thin devices with designed properties. To achieve a high density, bottom-up integration, the growth of these 2D heterostructures via van der Waals epitaxy (vdWE) is an attractive alternative to the currently mostly employed mechanical transfer, which is still problematic in terms of scaling and reproducibility. However, controlling the location of the nuclei formation remains a key challenge in vdWE. Here, we use a focused He ion beam for a deterministic placement of defects in graphene …
Universal effect of ammonia pressure on synthesis of colloidal metal nitrides in molten salts
Pritzker School of Molecular Engineering, University of Chicago（芝加哥大学普里茨克分子工程学院）；Interdisciplinary Materials Science Program, Vanderbilt University（范德堡大学交叉材料科学项目）；Department of Chemistry and James Franck Institute, University of Chicago（芝加哥大学化学系和詹姆斯·弗兰克研究所）；Department of Chemistry, Northwestern University（西北大学化学系）；Center for Nanoscale Materials, Argonne National Laboratory（阿贡国家实验室纳米材料中心）；Department of Chemical and Biomolecular Engineering, Vanderbilt University（范德堡大学化学与生物分子工程系）
The control over impurities like hydrogen and oxygen is of key importance in nitride-based semiconducting due to their unrivaled applicability in optoelectronics and high power/high frequency electronics. Therefore, it is desirable to continue the research on its diffusion and segregation in semiconductor materials. In this work, we report on a first observation on hydrogen outdiffusion from bulk crystalline gallium nitride. The extent of the hydrogen diffusion is established by secondary ion mass spectrometry. Analysis of characteristic hydrogen profile in GaN grown using ammonothermal method…
