Mississippi State University
Arnoldus, Henk F.
Foley, John T.
Other Advisors or Committee Members
Miller, Vivien G.
Date of Degree
Dissertation - Open Access
In this dissertation, we study the electronic and geometric structure of semiconductors and metal surfaces based on quantum mechanical first-principles calculations. We determine the geometry of vacancy defects of hydrogen adsorbed on a Pd(111) surface by treating the motion of a hydrogen atom, in addition to electrons, quantum mechanically. The calculated ground state wave function has high probability density in the hcp site located at the center of the vacancy instead of the fcc sites where the potential is minimum and hydrogen atoms on a Pd(111) surface normally adsorb. The geometry of quantum mechanically determined divacancy provides a simple and clear explanation for the scanning tunneling microscopy (STM) images of these defects that appear as three-lobed objects as observed in recent experiments [Mitsui, et al, Nature 422, 705 (2003)]. We employ the same principle to successfully elucidate the STM images of larger size vacancy defects. Our model also provides a compelling argument to explain the unusual recent experimental result that aggregates of three or more hydrogen vacancies are much more active in adsorption of hydrogen molecules while two-vacancy defects are never inactive. The InAs (110) surfaces appear lower than GaSb in STM images. This height difference is caused primarily by differences in the electronic structure of the two materials according to our calculations in a good agreement with measurements. In contrast, local variations in the apparent height of (110) surface atoms at InSb- or GaAs-like interfaces arise primarily from geometric distortions associated with local differences in bond length. The arsenic atoms adsorb preferably at the bridge sites between the dimerized Sb atoms on Sb-terminating (001) surfaces. Indium atoms, on the other hand, have somewhat equal probabilities at a few different sites on Ga-terminating (001) surfaces. Our calculated energies for atomic intermixing indicate that anion exchanges are exothermic for As atoms on Ga-terminating (001) interfaces but endothermic for In atoms on Sb-terminating (001) interfaces. This difference may explain why GaAs interfaces are typically more disordered than InSb interfaces in these heterostructures.
Kim, Sungho, "First-Principles Study Of Semiconductor And Metal Surfaces" (2005). Theses and Dissertations MSU. 2302.