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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Control of polymorphism during epitaxial growth of hyperferroelectric candidate LiZnSb on GaSb (111)B

A major challenge for ferroelectric devices is the depolarization field, which competes with and often destroys long-range polar order in the limit of ultrathin films. Recent theoretical predictions suggest a new class of materials, termed hyperferroelectics, that should be robust against the depolarization field and enable ferroelectricity down to the monolayer limit. Here, the authors demonstrate the epitaxial growth of hexagonal LiZnSb, one of the hyperferroelectric candidate materials, by molecular-beam epitaxy on GaSb (111)B substrates. Due to the high volatility of all three atomic species, they find that LiZnSb can be grown in an adsorption-controlled window, using an excess zinc flux. Within this window, the desired polar hexagonal phase is stabilized with respect to a competing cubic polymorph, as revealed by x-ray diffraction and transmission electron microscopy measurements. First-principles calculations show that for moderate amounts of epitaxial strain and moderate concentrations of Li vacancies, the cubic LiZnSb phase is lower in formation energy than the hexagonal phase, but only by a few millielectronvolts per formula unit. Therefore, they suggest that kinetics plays a role in stabilizing the desired hexagonal phase at low temperatures. Their results provide a path toward experimentally demonstrating ferroelectricity and hyperferroelectricity in a new class of ternary intermetallic compounds.

42 ENGINEERING↗
DOE OSTI2021

High-power narrow spectrum GaSb-based DBR lasers emitting near 2.1 µm

Stable high-power narrow-linewidth operation of the 2.05–2.1 µm GaSb-based diode lasers was achieved by utilizing the sixth-order surface-etched distributed Bragg reflector (DBR) mirrors. The DBR multimode devices with 100 µm wide ridge waveguides generated ~850 mW in the continuous wave (CW) regime at 20°C. The device CW output power was limited by thermal rollover. The laser emission spectrum was defined by Bragg reflector reflectivity at all operating currents in a wide temperature range. Finally, the devices operated at DBR line with detuning from gain peak exceeding 10 meV.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Optical and electrical properties of proton-implanted p -GaSb for electrical isolation

The effect of proton implantation as isolation implant and subsequent annealing on the optical absorption and electrical resistivity of low-bandgap p -GaSb is reported. The measured transmittance spectra indicates that implantation creates a distribution of energy levels extending into the bandgap. Electrical measurements show that the average sheet resistance of the implanted layer increases only by an order of magnitude from its pre-implantation value at a proton dose of ~10 13 cm -2 followed by 200 °C annealing. It is also shown that annealing reduces the implantation-induced optical absorption while still retaining a high electrical resistivity.

42 ENGINEERING↗
DOE OSTI2020

Materials Data on Ba(GaSb)2 by Materials Project

BaGa2Sb2 crystallizes in the orthorhombic Pnma space group. The structure is three-dimensional. there are two inequivalent Ba2+ sites. In the first Ba2+ site, Ba2+ is bonded in a 6-coordinate geometry to six Sb3- atoms. There are a spread of Ba–Sb bond distances ranging from 3.58–3.83 Å. In the second Ba2+ site, Ba2+ is bonded in a 6-coordinate geometry to six Sb3- atoms. There are a spread of Ba–Sb bond distances ranging from 3.57–3.69 Å. There are four inequivalent Ga2+ sites. In the first Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three equivalent Sb3- atoms. There are two shorter (2.75 Å) and one longer (2.85 Å) Ga–Sb bond lengths. In the second Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are two shorter (2.73 Å) and one longer (2.82 Å) Ga–Sb bond lengths. In the third Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are one shorter (2.70 Å) and two longer (2.75 Å) Ga–Sb bond lengths. In the fourth Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are one shorter (2.74 Å) and two longer (2.77 Å) Ga–Sb bond lengths. There are four inequivalent Sb3- sites. In the first Sb3- site, Sb3- is bonded in a 7-coordinate geometry to four Ba2+ and three Ga2+ atoms. In the second Sb3- site, Sb3- is bonded in a 5-coordinate geometry to two equivalent Ba2+ and three Ga2+ atoms. In the third Sb3- site, Sb3- is bonded to three equivalent Ba2+ and three Ga2+ atoms to form distorted edge-sharing SbBa3Ga3 octahedra. In the fourth Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Ba2+ and three equivalent Ga2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Materials Data on Eu(GaSb)2 by Materials Project

EuGa2Sb2 crystallizes in the triclinic P1 space group. The structure is three-dimensional. there are four inequivalent Eu2+ sites. In the first Eu2+ site, Eu2+ is bonded in a 6-coordinate geometry to six Sb3- atoms. There are a spread of Eu–Sb bond distances ranging from 3.39–3.47 Å. In the second Eu2+ site, Eu2+ is bonded in a 6-coordinate geometry to six Sb3- atoms. There are a spread of Eu–Sb bond distances ranging from 3.41–3.48 Å. In the third Eu2+ site, Eu2+ is bonded in a 6-coordinate geometry to six Sb3- atoms. There are a spread of Eu–Sb bond distances ranging from 3.39–3.47 Å. In the fourth Eu2+ site, Eu2+ is bonded in a 6-coordinate geometry to six Sb3- atoms. There are a spread of Eu–Sb bond distances ranging from 3.40–3.47 Å. There are eight inequivalent Ga2+ sites. In the first Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. All Ga–Sb bond lengths are 2.72 Å. In the second Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. All Ga–Sb bond lengths are 2.72 Å. In the third Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. All Ga–Sb bond lengths are 2.72 Å. In the fourth Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. All Ga–Sb bond lengths are 2.72 Å. In the fifth Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are two shorter (2.73 Å) and one longer (2.86 Å) Ga–Sb bond lengths. In the sixth Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are a spread of Ga–Sb bond distances ranging from 2.72–2.86 Å. In the seventh Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are two shorter (2.73 Å) and one longer (2.87 Å) Ga–Sb bond lengths. In the eighth Ga2+ site, Ga2+ is bonded in a trigonal non-coplanar geometry to three Sb3- atoms. There are a spread of Ga–Sb bond distances ranging from 2.72–2.87 Å. There are eight inequivalent Sb3- sites. In the first Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the second Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the third Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the fourth Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the fifth Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the sixth Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the seventh Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms. In the eighth Sb3- site, Sb3- is bonded in a 6-coordinate geometry to three Eu2+ and three Ga2+ atoms.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Carrier recombination dynamics and temperature dependent optical properties of InAs–GaSb heterostructures

Heterostructures with two dissimilar materials could offer unprecedented properties if one can carefully synthesize these heterostructures with atomically smooth interfaces and reduced number of recombination centers. InAs/GaSb-based heterostructures have technological importance for long wavelength infrared photodetectors if one can synthesize these materials with high-optical quality and high-carrier lifetime. In this work, the InAs/GaSb heterostructures with a different number of heterointerfaces and growth conditions were grown by solid source molecular beam epitaxy using valved cracker sources for both arsenic and antimony. Precise control of growth parameters and shutter sequences enabled abrupt InAs/GaSb heterointerfaces, as supported by a high-resolution transmission electron microscopic study. The temperature and power-dependent optical properties by photoluminescence (PL) spectroscopic analysis of InAs/GaSb heterostructures with 4 and 28 heterointerfaces displayed donor to the acceptor and the exciton bound to complex defects (V Ga Ga Sb ) 0 . Since the optical transition in PL measurements serves to determine the quality of the material, and the observed excitonic transitions from these InAs/GaSb heterostructures is an indication of high-quality materials. The high-carrier lifetimes of 139 ns to 185 ns from InAs/GaSb heterostructures were measured using microwave photoconductivity decay (μ-PCD) technique at room temperature. The observed increase in carrier lifetime is due to the decreasing number of Ga-related carrier recombination centers or defect complexes. This is further supported by the PL spectroscopic study. In addition, the carrier lifetime with different injection levels is supported by Shockley–Read–Hall recombination. We report these InAs/GaSb heterostructures with high-optical quality and high-carrier lifetimes would offer a path for the development of high-performance infrared photodetectors.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Structural anisotropy in Sb thin films

Sb thin films have attracted wide interest due to their tunable band structure, topological phases, high electron mobility, and thermoelectric properties. We successfully grow epitaxial Sb thin films on a closely lattice-matched GaSb(001) surface by molecular beam epitaxy. We find a novel anisotropic directional dependence on their structural, morphological, and electronic properties. The origin of the anisotropic features is elucidated using first-principles density functional theory (DFT) calculations. The growth regime of crystalline and amorphous Sb thin films was determined by mapping the surface reconstruction phase diagram of the GaSb(001) surface under Sb 2 flux, with confirmation of structural characterizations. Crystalline Sb thin films show a rhombohedral crystal structure along the rhombohedral (211) surface orientation parallel to the cubic (001) surface orientation of the GaSb substrate. At this coherent interface, Sb atoms are aligned with the GaSb lattice along the [1̄10] crystallographic direction but are not aligned well along the [110] crystallographic direction, which results in anisotropic features in reflection of high-energy electron diffraction patterns, misfit dislocation formation, surface morphology, and transport properties. Our DFT calculations show that the preferential orientation of the rhombohedral Sb (211) plane may originate from the GaSb surface, where Sb atoms align with the Ga and Sb atoms on the reconstructed surface. The formation energy calculations confirm the stability of the experimentally observed structures. Our results provide optimal film growth conditions for further studies of novel properties of Bi 1-x Sb x thin films with similar lattice parameters and an identical crystal structure, as well as functional heterostructures of them with III–V semiconductor layers along the (001) surface orientation, supported by a theoretical understanding of the anisotropic film orientation.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Tunable Mid-Infrared Interband Emission from Tensile-Strained InGaAs Quantum Dots

We demonstrate the ability to tailor self-assembled growth of In 0.5 Ga 0.5 As quantum dots (QDs) on GaSb(111)A surfaces by molecular beam epitaxy. Spontaneous formation via the Volmer–Weber growth mode produces QDs with excellent structural and optical quality. By harnessing tensile strain to reduce their band gap energy, these QDs are characterized by light emission that extends into the midwave infrared wavelength range of 3.2–3.9 μm (0.318–0.388 eV). As we increase QD size, we can tune the band alignment from type-III to type-II, where light emission occurs due to interband recombination between quantum confined electrons in the InGaAs QDs and holes in the GaSb barriers. Of particular interest is an unusual blue-shift in emission wavelength with increasing QD size, which we attribute to the incorporation of Sb into the InGaAs QDs from the GaSb barriers. By expanding this approach to produce tensile-strained QDs from other narrow band gap semiconductors, we anticipate the development of a range of highly tunable mid-infrared light sources.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Spinor $GW$ Bethe-Salpeter calculations in BerkeleyGW: Implementation, symmetries, benchmarking, and performance

Computing the GW quasiparticle band structure and Bethe-Salpeter equation (BSE) absorption spectra for materials with spin-orbit coupling have commonly been done by treating GW corrections and spin-orbit coupling (SOC) as separate perturbations to density-functional theory. However, accurate treatment of materials with strong spin-orbit coupling (such as many topological materials of recent interest, and thermoelectrics) often requires a nonperturbative approach using spinor wave functions in the Kohn-Sham equation and GW/BSE. Such calculations have only recently become available, in particular for the BSE. Here, we have implemented this approach in the plane-wave pseudopotential GW/BSE code BerkeleyGW, which is highly parallelized and widely used in the electronic-structure community. We present reference results for quasiparticle band structures and optical absorption spectra of solids with different strengths of spin-orbit coupling, including Si, Ge, GaAs, GaSb, CdSe, Au, and Bi 2 Se 3 . The calculated quasiparticle band gaps of these systems are found to agree with experiment to within a few tens of meV. SOC splittings are found to be generally in better agreement with experiment, including quasiparticle corrections to band energies. The absorption spectrum of GaAs is not significantly impacted by the inclusion of spin-orbit coupling due to its relatively small value (0.2 eV) in the Λ direction, while the absorption spectrum of GaSb calculated with the spinor GW/BSE captures the large spin-orbit splitting of peaks in the spectrum. For the prototypical topological insulator Bi 2 Se 3 , we find a drastic change in the low-energy band structure compared to that of DFT, with the spinorial treatment of the GW approximation correctly capturing the parabolic nature of the valence and conduction bands after including off-diagonal self-energy matrix elements. We present the detailed methodology, approach to spatial symmetries for spinors, comparison against other codes, and performance compared to spinless GW/BSE calculations and perturbative approaches to SOC. This work aims to spur further development of spinor GW/BSE methodology in excited-state research software and enables a more accurate and detailed exploration of electronic and optical properties of materials containing elements with large atomic numbers.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Consideration of temperature-dependent emissivity of selective emitters in thermophotovoltaic systems

Spectral emissivity control is paramount for designing a high-efficiency selective emitter surface required for thermophotovoltaic (TPV) applications. Owing to the temperature dependency of materials optical constants, the spectral properties of a selective emitter surface changes with the emitter temperature. This paper presents the fabrication of a multilayer metal-dielectric ( ${\rm Si}_{3}{\rm N}_{4}/\rm W/Si_{3}{\rm N_{4}}$ ) coated tungsten selective emitter aimed for GaSb-based TPV systems and studies the dependence of its surface spectral emissivity, $\varepsilon (\lambda)$ , upon a temperature ranging from 300 K to 1500 K. Both the simulation and experimental methods were used to characterize $\varepsilon (\lambda)$ as a function of temperature. For wavelengths less than 1.4 µm, $\varepsilon (\lambda)$ was found to have a minimal dependence on temperature. Beyond 1.4 µm, $\varepsilon (\lambda)$ increases with the temperature. At 1.55 µm, the simulation and experimental data estimated a ${\sim}{{4}}\%$ greater emissivity at 1500 K than at room temperature. At 1500 K, the increased $\varepsilon (\lambda)$ at longer wavelengths lowered the spectral conversion efficiency of the selective emitter from 58% to 47%. The output power density, sub-bandgap loss, and TPV conversion efficiency ( ${\eta _{\rm TPV}}$ ) for a GaSb cell illuminated by the selective thermal emitter at 1500 K were estimated. ${\eta _{\rm TPV}}$ drops from 13.7% to 11% due to the increased sub-bandgap emission at 1500 K. Essential approaches for mitigating the sub-bandgap losses to further improve ${\eta _{\rm TPV}}$ are also discussed.

42 ENGINEERING↗
DOE OSTI2024

Edge majorana quasiparticles and qubits

Various embodiments described herein provide for a topological quantum computer that uses edge Majorana quasi-particles to form qubits. An inverted Indium Arsenide (InAs) and Gallium Antimonide (GaSb) heterostructure is disclosed that is a quantum spin Hall insulator. A layer of aluminum can be deposited over a nanotube that is placed across the layers of the heterostructure. Once the nanotube is removed, and a gate is formed on the heterostructure and the heterostructure is cooled so that the aluminum becomes superconducting, helical edge states are formed at the junction of the super conducting aluminum, the InAs, and the GaSb which creates a Majorana zero modes (MZMs) at zero magnetic field. The MZMs can be used to construct a topological qubit for fault-resistant topological quantum computation.

Pan, Wei↗
DOE OSTI2020

Dual-Wavelength Y-Branch DBR Lasers With 100 mW of CW Power Near 2 μm

In this study, the interband GaSb-based diode lasers emitting simultaneously in two narrow bands separated by either ~1.6 or ~3.3 THz were designed, fabricated and characterized. The device active region contained one asymmetric tunnel-coupled double quantum well with separation between two lowest electron subbands controlled by thickness of the tunnel barrier. The Y-branch 6th order distributed Bragg reflector devices have been fabricated with either deep or shallow etched ridge waveguides. The increase of the deeply etched ridge waveguide width from 10 to 20 μm improved laser threshold and efficiency thanks to reduction of the relative role of the sidewall defect recombination. Further improvement of the device performance parameter was achieved by shallow etching. The shallow etched lasers with stable dual-wavelength emission spectrum generated 100 mW of continuous wave output power at 20 °C

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

The Role of Optical Phonon Confinement in the Infrared Dielectric Response of III–V Superlattices

Polar dielectrics are key materials of interest for infrared (IR) nanophotonic applications due to their ability to host phonon-polaritons that allow for low-loss, subdiffractional control of light. The properties of phonon-polaritons are limited by the characteristics of optical phonons, which are nominally fixed for most “bulk” materials. Superlattices composed of alternating atomically thin materials offer control over crystal anisotropy through changes in composition, optical phonon confinement, and the emergence of new modes. In particular, the modified optical phonons in superlattices offer the potential for so-called crystalline hybrids whose IR properties cannot be described as a simple mixture of the bulk constituents. To date, however, studies have primarily focused on identifying the presence of new or modified optical phonon modes rather than assessing their impact on the IR response. Here, this study focuses on assessing the impact of confined optical phonon modes on the hybrid IR dielectric function in superlattices of GaSb and AlSb. Using a combination of first principles theory, Raman, FTIR, and spectroscopic ellipsometry, the hybrid dielectric function is found to track the confinement of optical phonons, leading to optical phonon spectral shifts of up to 20 cm -1 . These results provide an alternative pathway toward designer IR optical materials.

36 MATERIALS SCIENCE↗