Matching Items (2)
Filtering by
- All Subjects: Semiconductors
- Member of: ASU Electronic Theses and Dissertations
Description
The structural and electronic properties of compositionally complex semiconductors have long been of both theoretical interest and engineering importance. As a new class of materials with an intrinsic compositional complexity, medium entropy alloys (MEAs) are immensely studied mainly for their excellent mechanical properties. The electronic properties of MEAs, however, are less well investigated. In this thesis, various properties such as electronic, spin, and thermal properties of two three-dimensional (3D) and two two-dimensional (2D) compositionally complex semiconductors are demonstrated to have promising various applications in photovoltaic, thermoelectric, and spin quantum bits (qubits).3D semiconducting Si-Ge-Sn and C3BN alloys is firstly introduced. Density functional theory (DFT) calculations and Monte Carlo simulations show that the Si1/3Ge1/3Sn1/3 MEA exhibits a large local distortion effect yet no chemical short-range order. Single vacancies in this MEA can be stabilized by bond reformations while the alloy retains semiconducting. DFT and molecular dynamics calculations predict that increasing the compositional disorder in SiyGeySnx MEAs enhances their electrical conductivity while weakens the thermal conductivity at room temperature, making the SiyGeySnx MEAs promising functional materials for thermoelectric devices. Furthermore, the nitrogen-vacancy (NV) center analog in C3BN (NV-C3BN) is studied to explore its applications in quantum computers. This analog possesses similar properties to the NV center in diamond such as a highly localized spin density and strong hyperfine interactions, making C3BN suitable for hosting spin qubits. The analog also displays two zero-phonon-line energies corresponding to wavelengths close to the ideal telecommunication band width, useful for quantum communications.
2D semiconducting transition metal chalcogenides (TMCs) and PtPN are also investigated. The quaternary compositionally complex TMCs show tunable properties such as in-plane lattice constants, band gaps, and band alignment, using a high through-put workflow from DFT calculations in conjunction with the virtual crystal approximation. A novel 2D semiconductor PtPN of direct bandgap is also predicted, based on pentagonal tessellation.
The work in the thesis offers guidance to the experimental realization of these novel semiconductors, which serve as valuable prototypes of other compositionally complex systems from other elements.
2D semiconducting transition metal chalcogenides (TMCs) and PtPN are also investigated. The quaternary compositionally complex TMCs show tunable properties such as in-plane lattice constants, band gaps, and band alignment, using a high through-put workflow from DFT calculations in conjunction with the virtual crystal approximation. A novel 2D semiconductor PtPN of direct bandgap is also predicted, based on pentagonal tessellation.
The work in the thesis offers guidance to the experimental realization of these novel semiconductors, which serve as valuable prototypes of other compositionally complex systems from other elements.
ContributorsWang, Duo (Author) / Zhuang, Houlong (Thesis advisor) / Singh, Arunima (Committee member) / Jiao, Yang (Committee member) / Arizona State University (Publisher)
Created2020
Description
Single-layer pentagonal materials have received limited attention compared with their counterparts with hexagonal structures. They are two-dimensional (2D) materials with pentagonal structures, that exhibit novel electronic, optical, or magnetic properties. There are 15 types of pentagonal tessellations which allow plenty of options for constructing 2D pentagonal lattices. Few of them have been explored theoretically or experimentally. Studying this new type of 2D materials with density functional theory (DFT) will inspire the discovery of new 2D materials and open up applications of these materials in electronic and magnetic devices.In this dissertation, DFT is applied to discover novel 2D materials with pentagonal structures. Firstly, I examine the possibility of forming a 2D nanosheet with the vertices of type 15 pentagons occupied by boron, silicon, phosphorous, sulfur, gallium, germanium or tin atoms. I obtain different rearranged structures such as a single-layer gallium sheet with triangular patterns. Then the exploration expands to other 14 types of pentagons, leading to the discoveries of carbon nanosheets with Cairo tessellation (type 2/4 pentagons) and other patterns. The resulting 2D structures exhibit diverse electrical properties. Then I reveal the hidden Cairo tessellations in the pyrite structures and discover a family of planar 2D materials (such as PtP2), with a chemical formula of AB2 and space group pa ̄3. The combination of DFT and geometries opens up a novel route for the discovery of new 2D materials. Following this path, a series of 2D pentagonal materials such as 2D CoS2 are revealed with promising electronic and magnetic applications. Specifically, the DFT calculations show that CoS2 is an antiferromagnetic semiconductor with a band gap of 2.24 eV, and a N ́eel temperature of about 20 K. In order to enhance the superexchange interactions between the ions in this binary compound, I explore the ternary 2D pentagonal material CoAsS, that lacks the inversion symmetry. I find out CoAsS exhibits a higher Curie temperature of 95 K and a sizable piezoelectricity (d11=-3.52 pm/V). In addition to CoAsS, 34 ternary 2D pentagonal materials are discovered, among which I focus on FeAsS, that is a semiconductor showing strong magnetocrystalline anisotropy and sizable Berry curvature. Its magnetocrystalline anisotropy energy is 440 μeV/Fe ion, higher than many other 2D magnets that have been found.
Overall, this work not only provides insights into the structure-property relationship of 2D pentagonal materials and opens up a new route of studying 2D materials by combining geometry and computational materials science, but also shows the potential applications of 2D pentagonal materials in electronic and magnetic devices.
Overall, this work not only provides insights into the structure-property relationship of 2D pentagonal materials and opens up a new route of studying 2D materials by combining geometry and computational materials science, but also shows the potential applications of 2D pentagonal materials in electronic and magnetic devices.
ContributorsLiu, Lei (Author) / Zhuang, Houlong (Thesis advisor) / Singh, Arunima (Committee member) / Jiao, Yang (Committee member) / Arizona State University (Publisher)
Created2020