Correction: Atomate2: modular workflows for materials science
[This corrects the article DOI: 10.1039/D5DD00019J.].
Ganose, Alex M↗
Engineering topics
Biswas, Tathagata
Publications and source records attributed to Biswas, Tathagata.
Electronic Properties of Ultra‐Wide Bandgap B x Al 1− x N Computed from First‐Principles Simulations
Abstract Ultra‐wide bandgap (UWBG) materials such as AlN and BN hold great promise for future power electronics due to their exceptional properties. They exhibit large bandgaps, high breakdown fields, high thermal conductivity, and high mechanical strengths. AlN and BN have been extensively researched, however, their alloys, B x Al 1− x N, are much less studied despite their ability to offer tunable properties by adjusting x . In this article, the electronic properties of 17 recently predicted ground states of B x Al 1− x N in the x = 0 − 1 range are predicted using first‐principles density functional theory and many‐body perturbation theory within GW approximation. All the B x Al 1− x N structures are found to be UWBG materials and have bandgaps that vary linearly from that of wurtzite‐phase ( w ) AlN (6.19 eV) to that of w ‐BN (7.47 eV). The bandstructures of B x Al 1− x N show that a direct‐to‐indirect bandgap crossover occurs near x = 0.25. Furthermore, it is found that B x Al 1− x N alloys have much larger dielectric constants than the constituent bulk materials (AlN = 9.3 ɛ 0 or BN = 7.3 ɛ 0 ), with values reaching as high as 12.1 ɛ 0 . These alloys are found to exhibit large dielectric breakdown fields in the range 9–35 MV cm −1 with a linear dependence on x . This work provides the much needed advancement in the understanding of the properties of B x Al 1− x N to aid their application in next‐generation devices.
Milne, Cody L.↗
Ab Initio Prediction of Ultra‐Wide Band Gap B x Al 1− x N Materials
Abstract Ultra‐wide bandgap (UWBG) materials are poised to play an important role in the future of power electronics. Devices made from UWBG materials are expected to operate at higher voltages, frequencies, and temperatures than current silicon and silicon‐carbide‐based devices and can even lead to significant miniaturization of such devices. In the UWBG field, aluminum nitride and boron nitride have attracted great interest; however, the B x Al 1− x N alloys are much less studied. In this work, using first‐principles simulations combining density‐functional theory and the cluster expansion method, the crystal structure of B x Al 1− x N alloys is predicted. Seventeen ground state structures of B x Al 1− x N with formation energies between 0.11 and 0.25 eV atom ‐1 are found. All of these structures are found to be dynamically stable. The B x Al 1− x N structures are found to have predominantly a tetrahedral bonding environment; however, some structures exhibit sp 2 bonds similar to hexagonal BN. This work expands knowledge of the structures, energies, and bonding in B x Al 1− x N which aids their synthesis, the innovation of lateral or vertical devices, and discovery of compatible dielectric and Ohmic contact materials.
36 MATERIALS SCIENCE↗
pyGWBSE: a high throughput workflow package for GW-BSE calculations
Abstract We develop an open-source python workflow package, py GWBSE to perform automated first-principles calculations within the GW-BSE (Bethe-Salpeter) framework. GW-BSE is a many body perturbation theory based approach to explore the quasiparticle (QP) and excitonic properties of materials. GW approximation accurately predicts bandgaps of materials by overcoming the bandgap underestimation issue of the more widely used density functional theory (DFT). BSE formalism produces absorption spectra directly comparable with experimental observations. py GWBSE package achieves complete automation of the entire multi-step GW-BSE computation, including the convergence tests of several parameters that are crucial for the accuracy of these calculations. py GWBSE is integrated with Wannier90 , to generate QP bandstructures, interpolated using the maximally-localized wannier functions. py GWBSE also enables the automated creation of databases of metadata and data, including QP and excitonic properties, which can be extremely useful for future material discovery studies in the field of ultra-wide bandgap semiconductors, electronics, photovoltaics, and photocatalysis.
36 MATERIALS SCIENCE↗
Excitonic effects in absorption spectra of carbon dioxide reduction photocatalysts
Abstract The formation and disassociation of excitons play a crucial role in any photovoltaic or photocatalytic application. However, excitonic effects are seldom considered in materials discovery studies due to the monumental computational cost associated with the examination of these properties. Here, we study the excitonic properties of nearly 50 photocatalysts using state-of-the-art Bethe–Salpeter formalism. These ~50 materials were recently recognized as promising photocatalysts for CO 2 reduction through a data-driven screening of 68,860 materials. Here, we propose three screening criteria based on the optical properties of these materials, taking excitonic effects into account, to further down select six materials. Furthermore, we study the correlation between the exciton binding energies obtained from the Bethe–Salpeter formalism and those obtained from the computationally much less-expensive Wannier–Mott model for these chemically diverse ~50 materials. This work presents a paradigm towards the inclusion of excitonic effects in future materials discovery for solar-energy harvesting applications.
36 MATERIALS SCIENCE↗
Two-dimensional forms of robust CO 2 reduction photocatalysts
Photoelectrocatalysts that use sunlight to power the CO 2 reduction reaction will be crucial for carbon-neutral power and energy-efficient industrial processes. Scalable photoelectrocatalysts must satisfy a stringent set of criteria, such as stability under operating conditions, product selectivity, and efficient light absorption. Two-dimensional materials can offer high specific surface area, tunability, and potential for heterostructuring, providing a fresh landscape of candidate catalysts. From a set of promising bulk CO 2 reduction photoelectrocatalysts, we screen for candidate monolayers of these materials, then study their catalytic feasibility and suitability. For stable monolayer candidates, we verify the presence of visible-light band gaps, check that band edges can support CO 2 reduction, determine exciton binding energies, and compute surface reactivity. We find visible light absorption for SiAs, ZnTe, and ZnSe monolayers, and that due to a lack of binding, CO selectivity is possible. We thus identify SiAs, ZnTe, and ZnSe monolayers as targets for further investigation, expanding the chemical space for CO 2 photoreduction candidates.
36 MATERIALS SCIENCE↗
Polarization discontinuity driven two dimensional electron gas at A2Mo3O8/B2Mo3O8 (A, B: Zn, Mg, Cd) interfaces
Not Available
Biswas, Tathagata↗
Electrical and optical properties of low-bandgap oxide Zn 2 Mo 3 O 8 for optoelectronic applications
Semiconducting metal oxides are attractive for various applications since most oxides are non-toxic, stable, and easy to deposit. Wide band-gap materials have been studied more extensively, compared to low bandgap materials, which introduces limitations to the applications of oxides. Study of low band-gap semiconducting oxides can propel the usage of oxides in a wider range of applications. The electronic, structural, and optical properties of Zn 2 Mo 3 O 8 (ZMO) are investigated. Stoichiometric polycrystalline films of ZMO are deposited using pulsed laser deposition system at room temperature. The unintentionally n-doped films show a hall electron mobility of 0.7 cm 2 V -1 s -1 and have a bandgap of 2.1 eV. The photoelectron spectra contain complex peak profiles which are explained to be a manifestation of final state effects. The orbital contribution to the valence band of ZMO is probed using resonant photoelectron spectroscopy, which confirms that the valence band is composed of Mo 4d levels. The conduction and valence band edges are predicted to be at 4.2 eV and 6.3 eV, so most of the conventional wide band-gap oxides can be used as hole-blocking layers with ZMO. Under A.M. 1.5 illumination, single-sided Schottky diode with Fluorine-doped tin oxide/TiO 2 /ZMO/Au structure shows no photovoltaic action, possibly due to high exciton binding energy and low carrier drift lengths. However, the Schottky device shows a higher current under illumination, which suggests that with improvement in carrier drift lengths, ZMO can find applications in low-cost optoelectronic devices on flexible substrates like plastic or Polyethylene terephthalate.
36 MATERIALS SCIENCE↗