Hosted by: Mark Hybertsen

First-principles quantum mechanical methods, e.g. density functional theory (DFT) and correlated wavefunction theories, have made possible accurate theoretical description of chemical processes such as chemical bond-breaking and forming, and charge transfer. To be able to describe surface processes on metal and metal oxides at the atomic level is of fundamental and practical interest because such processes give rise to or may affect macroscopic properties such as catalytic activity, chemical adsorption and absorption efficiency, and charge carrier conductivity, to name a few. The thermodynamics and kinetics of surface reconstruction in photocatalytic perovskite oxides, SrTiO3 and BaTiO3, are explored through DFT, and their implications for catalysis will be discussed. Secondly, the feasibility of light-driven catalysis on plasmonic metal nanoparticles (e.g., Au and Cu) will be presented. We studied the excited-state energetics of select heterogeneously catalyzed chemical reactions via the embedded correlated wavefunction method (e.g., multiconfigurational second order perturbation theory embedded in a density-functional-derived embedding potential). We evaluate if these excited-state reaction pathways are accessible via plasmon resonance and decay. N2 dissociation on Fe-doped Au(111) surface and CH4 activation on Ru-doped Cu(111) will be presented as examples.