Vibrational Signatures of Electronic Properties in Renewable-Energy Catalysis

The objective of this research program is to discover and develop new approaches for <em>ab initio</em> computational simulations of molecular motion. Specifically, this program aims to decipher the connection between the underlying electronic structure and the accordant molecular vibrations in reactive ions and radicals for renewable-energy purposes. Recent experimental progress in ion sources and optical spectroscopies has unearthed considerable new inner-sphere detail for these complexes, but the connection between these spectral signatures and mechanistic information often remains elusive, to the continued frustration of experimentalists. For this purpose, new anharmonic vibrational frequency methods, along with a publicly deployed software package, will be developed. Working closely with committed experimental collaborators, this conceptual and computational framework will be used to explain the results of new spectroscopy experiments, focusing specifically on the inner-shell mechanisms of renewable-energy catalysis. The oxidation half of catalytic water-splitting chemistry will be a central focus, along with fundamental studies of the manner in which strong ions and radicals activate solvent as a chemical species. The resulting products of the research program will include openly available software and algorithms for the <em>ab initio</em> simulation of challenging vibrational spectra, as well as critical mechanistic insight into energy-focused catalytic processes that are opaque to other existing analytical techniques.. Authors: Steele, Ryan P. [Univ. of Utah, Salt Lake City, UT (United States)]. DOE Contract: SC0019405. Subjects: 42 ENGINEERING; 74 ATOMIC AND MOLECULAR PHYSICS; 97 MATHEMATICS AND COMPUTING