The influence of Ga incorporation into cubic In$_2$O$_3$ on the electronic and vibrational properties is discussed for (In$_{1-x}$,Ga$_x$)$_2$O$_3$ alloy films grown by molecular beam epitaxy. Using spectroscopic ellipsometry, a linear dependence of the absorption onset on the Ga content $x$ is found with a blueshift of up to 150 meV for $x = 0.1$. Consistently, the fundamental band gap exhibits a blueshift as determined by hard X-ray photoelectron spectroscopy. The dependence of the absorption onset and the effective electron mass on the electron concentration is derived from the infrared dielectric functions for a Sn doped alloy film. The influence of alloying on phonon modes is analyzed on the basis of Raman spectroscopic measurements. The frequencies of several phonon modes are identified as sensitive measures for the spectroscopic determination of the Ga content.
Stubbed plates, i.e., thin elastic sheets endowed with pillar-like resonators, display subwavelength, locally-resonant bandgaps that are primarily controlled by the intrinsic resonance properties of the pillars. In this work, we experimentally study the bandgap response of a tunable heterogeneous plate endowed with reconfigurable families of pillars. We demonstrate that, under certain circumstances, both the spectrum of resonant frequencies of the pillars and their spatial arrangement influence the filtering characteristics of the system. Specifically, both spatially graded and disordered arra…
Halide double perovskites have gained significant attention, owing to their composition of low-toxicity elements, stability in air and long charge-carrier lifetimes. However, most double perovskites, including Cs2AgBiBr6, have wide bandgaps, which limit photo conversion efficiencies. The bandgap can be reduced through hallowing with Sb3+, but Sb-rich alloys are difficult to synthesise due to the high formation energy of Cs2AgSbBr6, which itself has a wide bandgap. We develop a solution-based route to synthesis phase-pure Cs2Ag(SbxBi1-x)Br6 thin films, with the mixing parameter x continuous var…
In this Letter, we demonstrate that it is possible to form a two-dimensional (2D) silicene-like Si$_5$Ge compound by replacing the Si atoms occupying on-top sites in the planar-like structure of epitaxial silicene on ZrB$_2$(0001) by deposited Ge atoms. For coverages below 1/6 ML, the Ge deposition gives rise to a Si$_{6-x}$Ge$_{x}$ alloy (with $x$ between 0 and 1) in which the on-top sites are randomly occupied by Si or Ge atoms. The progressive increase of the valence band maximum with $x$ observed experimentally originates from a selective charge transfer from Ge atoms to Si atoms. These ac…
The bowing of the energy of the three lowest band-to-band transitions in $β$-(Al$_{x}$Ga$_{1-x}$)$_2$O$_3$ alloys was resolved using a combined density functional theory (DFT) and generalized spectroscopic ellipsometry (GSE) approach. The DFT calculations of the electronic band structure of both, $β$-Ga$_2$O$_3$ and $θ$-Al$_2$O$_3$, allow extracting of the linear portion of the energy shift in the alloys, and provide a method for quantifying the role of coherent strain present in the $β$-(Al$_{x}$Ga$_{1-x}$)$_2$O$_3$ thin films on (010) $β$-Ga$_2$O$_3$ substrates. The energies of band-to-band …
The bandgap and band bowing parameter of semiconductor alloys are calculated with a fast and realistic approach. The method is a dielectric scaling approximation that is based on a scissor approximation. It adds an energy shift to the bandgap provided by the local density approximation (LDA) of the density functional theory (DFT). The energy shift consists of a material-independent constant weighted by the inverse of the high-frequency dielectric constant. The salient feature of the approach is the fast calculation of the dielectric constant of alloys via the Green function (GF) of the TB-LMTO…
Silicon crystallized in the usual cubic (diamond) lattice structure has dominated the electronics industry for more than half a century. However, cubic silicon (Si), germanium (Ge) and SiGe-alloys are all indirect bandgap semiconductors that cannot emit light efficiently. Accordingly, achieving efficient light emission from group-IV materials has been a holy grail in silicon technology for decades and, despite tremendous efforts, it has remained elusive. Here, we demonstrate efficient light emission from direct bandgap hexagonal Ge and SiGe alloys. We measure a subnanosecond, temperature-insen…
Monoclinic scheelite bismuth vanadate (BiVO4) is a promising photoanode for water splitting yet the PEC performance is limited due to its relatively higher (2.4 eV) band gap. Here, we successfully decreased its the band gap to 1.72 eV by controlled antimony alloying. Low bandgap antimony alloyed bismuth vanadium oxide (Sb:BiVO4) thin film was prepared by RF sputtering of high purity homemade target, fabricated by solid-state reaction using a mixture of Sb2O3, Bi2O3, and V2O5 powders with desired stoichiometric ratios. Several growth parameters, powder crystallography, post-deposition effects, …
Effect of Concentration Fluctuations on Material Properties of Disordered Alloys
Eastern Institute of Technology（东方理工大学）；Materials Department, University of California, Santa Barbara（加州大学圣塔芭芭拉分校材料系）；Beijing Computational Science Research Center（北京计算科学研究中心）
The electronic band structure of the (Ga,Mn)As system has been one of the most intriguing problems in solid state physics over the past two decades. Determination of the band structure evolution with increasing Mn concentration is a key issue to understand the origin of ferromagnetism. Here we present room temperature photoluminescence and ellipsometry measurements of Ga_{100%-x}Mn_{x}As alloy. The up-shift of the valence-band is proven by the red shift of the room temperature near band gap emission from the Ga_{100%-x}Mn_{x}As alloy with increasing Mn content. It is shown that even a doping b…
Electronic structures of Ge$_{1-x}$Sn$_{x}$ alloys (0 $\leq$ $x$ $\leq$ 1) are theoretically studied by nonlocal empirical pseudopotential method. For relaxed Ge$_{1-x}$Sn$_{x}$, a topological semimetal is found for $\textit x$ $>$ 41$\%$ with gapless and band inversion at $Γ$ point, while there is an indirect-direct bandgap transition at $x$ = 8.5$\%$. For strained Ge$_{1-x}$Sn$_{x}$ on a Ge substrate, semimetals with a negative indirect bandgap appear for $x$ $>$ 43$\%$, and the strained Ge$_{1-x}$Sn$_{x}$ on Ge is always an indirect bandgap semiconductor for $x$ $<$ 43$\%$. With appropriate…
Modification of graphene to open a robust gap in its electronic spectrum is essential for its use in field effect transistors and photochemistry applications. Inspired by recent experimental success in the preparation of homogeneous alloys of graphene and boron nitride (BN), we consider here engineering the electronic structure and bandgap of C$_{2x}$B$_{1-x}$N$_{1-x}$ alloys via both compositional and configurational modification. We start from the BN end-member, which already has a large bandgap, and then show that (a) the bandgap can in principle be reduced to about 2 eV with moderate subst…
Shining light on short-range atomic ordering in semiconductors alloys
Stanford University（斯坦福大学）；SLAC National Accelerator Laboratory（斯坦福直线加速器中心）；George Washington University（乔治华盛顿大学）；National Institute of Standards and Technology（美国国家标准与技术研究院）；University of California Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Max Planck Institute for Sustainable Materials（马克斯·普朗克可持续材料研究所）
Electrical and thermal transport properties of disordered materials have long been of both theoretical interest and engineering importance. As a new class of materials with an intrinsic compositional disorder, high/medium-entropy alloys (HEAs/MEAs) are being immensely studied mainly for their excellent mechanical properties. By contrast, electrical and thermal transport properties of HEAs/MEAs are less well studied. Here we investigate these two properties of silicon (Si)-germanium (Ge)-tin (Sn) MEAs, where we keep the same content of Si and Ge while increasing the content of Sn from 0 to 1/3 …
The energy position of the optical absorption edge and the free carrier populations in InxGa1-xN ternary alloys can be controlled using high energy 4He+ irradiation. The blue shift of the absorption edge after irradiation in In-rich material (x > 0.34) is attributed to the band-filling effect (Burstein-Moss shift) due to the native donors introduced by the irradiation. In Ga-rich material, optical absorption measurements show that the irradiation-introduced native defects are inside the bandgap, where they are incorporated as acceptors. The observed irradiation-produced changes in the optical …
The Hidden Cost of Alloying: Disorder-Driven Transport Collapse in TMDs
Dipartimento di Fisica Università della Calabria e INFN-gruppo collegato di Cosenza（卡拉布里亚大学物理系及科森扎INFN联合小组）；Instituto Madrileño de Estudios Avanzados, IMDEA Nanociencia（马德里高级研究院，IMDEA纳米科学研究所）；Departamento de Física de la Materia Condensada, Universidad Autónoma de Madrid（马德里自治大学凝聚态物理系）；Instituto de Física de la Materia Condensada IFIMAC, Univ. Autónoma de Madrid（马德里自治大学凝聚态物理研究所IFIMAC）；Walter Schottky Institute, Technical University of Munich（慕尼黑工业大学瓦尔特·肖特基研究所）；Catalan Institute of Nanoscience and Nanotechnology (ICN2),CSIC and BIST（加泰罗尼亚纳米科学与纳米技术研究所（ICN2），西班牙国家研究委员会和巴塞罗那理工大学）
Here, the structural, electronic and optical properties of the GaP1-xSbx/Si tandem materials association are determined in view of its use for solar water splitting applications. The GaPSb crystalline layer is grown on Si by Molecular Beam Epitaxy with different Sb contents. The bandgap value and bandgap type of GaPSb alloy are determined on the whole Sb range, by combining experimental absorption measurements with tight binding (TB) theoretical calculations. The indirect (X-band) to direct (Γ-band) cross-over is found to occur at 30% Sb content. Especially, at a Sb content of 32%, the GaP1-xS…
The unprecedented wide bandgap tunability (~1 eV) of Al$_x$In$_{1-x}$As$_y$Sb$_{1-y}$ latticed-matched to GaSb enables the fabrication of photodetectors over a wide range from near-infrared to mid-infrared. In this paper, the valence band-offsets in AlxIn1-xAsySb1-y with different Al compositions are analyzed by tight-binding calculations and X-ray photoelectron spectroscopy (XPS) measurements. The observed weak variation in valence band offsets is consistent with the lack of any minigaps in the valence band, compared to the conduction band.
We study the dielectric function of CuBr$_\mathrm{x}$I$_{1-\mathrm{x}}$ thin film alloys using spectroscopic ellipsometry in the spectral range between 0.7 eV to 6.4 eV, in combination with first-principles calculations based on density functional theory. Through the comparison of theory and experiment, we attribute features in the dielectric function to electronic transitions at specific k-points in the Brillouin zone. The observed bandgap bowing as a function of alloy composition is discussed in terms of different physical and chemical contributions. The band splitting at the top of the vale…
Ge-Sn alloys with a sufficiently high concentration of Sn is a direct bandgap group IV material. Recently, ion implantation followed by pulsed laser melting has been shown to be a promising method to realize this material due to its high reproducibility and precursor-free process. A Ge-Sn alloy with ~9 at.% Sn was shown to be feasible by this technique. However, the compressive strain, inherently occurring in heterogeneous epitaxy of the film, evidently delays the material from the direct bandgap transition. In this report, an attempt to synthesize a highly-relaxed Ge-Sn alloy will be presente…
Direct growth of crystalline spinel GaON films: A wide-bandgap mixed-anion semiconductor
State Key Laboratory of Radio Frequency Heterogeneous Integration, College of Physics and Optoelectronic Engineering, Shenzhen University（深圳大学物理与光电工程学院射频异构集成国家重点实验室）；Physics Department, The Hong Kong University of Science and Technology（香港科技大学物理系）
With the development of modern nanoscience and nanotechnology, Bi1-xSbx can be synthesized into different nanoscale and nanostructured forms, including thin films, nanowires, nanotubes, nanoribbons, and many others. However, due to the strong correlation between electrons and holes at the L-point in the Brillouin zone, the direct band evolves in an anomalous manner under the quantum confinement when nanostructured. Due to the alloying and the low symmetry, predicting the L-point direct bandgap in a nanomaterial using either ab initio calculations or kp perturbations can be computationally cost…
Effect of Annealing on Al Diffusion and its Impact on the Properties of Ga$_2$O$_3$ Thin Films Deposited on c-plane Sapphire by RF Sputtering
Instituto de Engenharia de Sistemas e Computadores — Microssistemas e Nanotecnologias (INESC MN)（计算机与系统工程学院—微系统与纳米技术研究所）；Instituto de Plasmas e Fusão Nuclear, Instituto Superior Técnico, Universidade de Lisboa（核聚变等离子体研究所，里斯本高等理工学院，里斯本大学）；Departamento de Física, Faculdade de Ciências, Universidade de Lisboa（理学院物理系，里斯本大学）；BioISI—Biosystems and Integrative Sciences Institute, Faculdade de Ciências, Universidade de Lisboa（生物与整合科学研究所，理学院，里斯本大学）；Centro de Química Estrutural, Institute of Molecular Sciences and Departamento de Engenharia Química, Instituto Superior Técnico, Universidade de Lisboa（结构化学中心，分子科学研究所，化学工程系，里斯本高等理工学院，里斯本大学）；Departamento de Engenharia e Ciências Nucleares, Instituto Superior Técnico（核科学与工程系，里斯本高等理工学院）
Beyond-diffraction-limit optical absorption spectroscopy provides profound information on the graded band structures of composition-spread and stacked two-dimensional materials, in which direct/indirect bandgap, interlayer coupling, sliding, and possible defects significantly modify their optoelectronic functionalities such as photoluminescence efficiency. We here visualize the spatially-varying band structure of monolayer and bilayer transition metal dichalcogenide alloys for the first time by using near-field broadband absorption microscopy. The near-field-spectral and -spatial diagrams mani…
Recently, Fang et al. have predicted a high ZT of 1.54 in TaSbRu alloys at 1200 K from first-principles without considering spin-orbit interaction, accurate electronic structure, details of phonon scattering, and energy-dependent holes relaxation time. Here, we report the details of structural stability and thermoelectric performance of Bi-Substituted p-type TaSbRu from first-principles calculations considering theses important parameters. This indirect bandgap semiconductor (Eg=0.8 eV by TB-mBJ+SOC) has highly dispersive and degenerate valence bands, which lead to a maximum power factor, 3.8 …
Low energy optical modes of MBE-grown In1-xGaxN thin films with different values of x are investigated using Raman spectroscopy. We also studied the influence of Raman excitation frequency using red and green lasers on scattering intensity of various Raman modes. For those In1-xGaxN alloys whose bandgap energy is close to the red laser, a huge enhancement in the intensities of A1(LO) mode and its 2A1(LO) replica is observed when excited with red laser as compared to the green laser excitation. We found that the energies of longitudinal optical modes (A1 (LO) and 2A1 (LO)) vary nonlinearly unli…
We have investigated the optical properties of thin films of topological insulators Bi$_{2}$Te$_{3}$, Bi$_{2}$Se$_{3}$ and their alloys Bi$_2$(Te$_{1-x}$Se$_x$)$_3$ on BaF$_{2}$ substrates by a combination of infrared ellipsometry and reflectivity in the energy range from 0.06 to 6.5 eV. For the onset of interband absorption in Bi$_2$Se$_3$, after the correction for the Burstein-Moss effect, we find the value of direct bandgap of $215\pm10$ meV at 10 K. Our data supports the picture that Bi$_2$Se$_3$ has a direct band gap located at the $Γ$ point in the Brillouin zone and that the valence band…
GeSn alloys are the subject of intense research activities as these group IV semiconductors present direct bandgap behaviors for high Sn contents. Today, the control of strain becomes an important challenge to improve GeSn devices. Strain micro-measurements are usually performed by Raman spectroscopy. However, different relationships linking the Raman spectral shifts to the built-in strain can be found in the literature. They were deduced from studies on low Sn content GeSn layers (i.e. xSn<8%) or on GeSiSn layers. In this work, we have calibrated the GeSn Raman relationship for really high Sn…
