Computational Discovery And Design Of Novel Single-Layer Materials For Electronic And Energy Applications
The last decade has seen an explosion of interest in two-dimensional materials, which now can be synthesized in either single or a few atomic layer forms. The discovery of novel fabrication methods for creating single-layer materials such as graphene, zinc oxide, silicon carbide, boron nitride, and molybdenum disulfide has opened a new field of materials research with promising applications for energy technologies. Single-layer materials not only represent the ultimate scaling in the vertical direction, but also show a variety of novel and useful electronic, optical, and mechanical properties. Using a data-mining and first-principles design approach we identify several previously unrecognized families of single-layer materials. We determine their energetic and dynamical stability, study their electronic and optical properties, and determine their suitability for electronic and energy applications using a combination of density-functional calculations with semi-local and hybrid density functionals, the many-body G0 W0 method, and the Bethe-Salpeter equation. To determine their suitability for photocatalytic water splitting we also determine their solubility in water. We discover several single-layer materials with promising properties for electronic devices such as for dielectric barriers in graphene field-effect tunneling transistors and for photocatalytic water splitting. Our results provide guidance for experimental synthesis efforts and future searches of materials suitable for applications in electronic device and energy technologies.
Single-layer materials; Density-functional theory; Semiconductors
Hennig, Richard G.
Schlom, Darrell; Muller, David Anthony
Materials Science and Engineering
Ph. D., Materials Science and Engineering
Doctor of Philosophy
dissertation or thesis