Computational Investigations into Plasmonic Excitations, Catalytic Reactions and Surface DopingPublic Deposited
The tools of computational chemistry allow researchers to gain insight into chemical systems that would be difficult or impossible to gain experimentally. This dissertation discusses the application of several of these computational tools to chemical systems of interest. First, we present several studies of plasmon resonance in Ag nanoclusters using time-dependent density functional theory. We demonstrate the effect of ligand-protection on plasmonic behavior, and then introduce a new method for identifying and analyzing plasmons in computational results and apply that method to a series of nanorod-like ligand-protected Ag clusters to study size-dependence of ligand effects. These studies afford us insight into optical properties for systems that would be nearly impossible to synthesize and measure experimentally. Second, we present a study of the possible reaction pathways for hydrogenation of CO on a Ni(110) surface, with and without the presence of subsurface hydrogen. This reaction pathway study allows us to look in detail at individual chemical processes that would be difficult or impossible to study experimentally. And finally, we present a study of surface doping of black phosphorus with Lewis acids, in which we predict the doping effects of a number of Lewis acid adsorbates and identify several promising candidates for further experimental study.