Charge transport, configuration interaction and Rydberg states under density functional theory

Abstract

Density functional theory (DFT) is a computationally efficient formalism for studying electronic structure and dynamics. In this work, we develop DFT-based excited-state methods to study electron transport, Rydberg excited states and to characterize diabatic electronic configurations and couplings. We simulate electron transport in a molecular wire using real-time time-dependent density functional theory in order to study the conduction of the wire. We also use constrained density functional theory to obtain diabatic states and diabatic couplings, and use these excited-state properties in a configuration-interaction method that treats both dynamic and static correlation. Lastly, we use eDFT, an excited-state self-consistent-field method, to determine the energies of excited Rydberg atomic states.