Modeling of non-equilibrium excited state processes in nanoscale systems create new challenges to time-domain density functional theory (TDDFT) and nonadiabatic molecular dynamics (NAMD). Examples include proper treatment of quantum coherence, transition from coherent to hopping transport in long-range charge and energy transfer, super-exchange, and many-particle Auger-type processes. Motivated by these challenges, our group developed several new NAMD techniques and implemented them within ab initio and tight-binding TDDFT. Decoherence-induced surface hopping (DISH) incorporates decoherence effects in a way that naturally achieves trajectory branching. Coherence penalty functional (CPF) uses DFT-like ideas to introduce decoherence into the Ehrenfest method. Self-consistent fewest-switches surface hopping (SC-FSSH) provides a simple solution to the trivial (or “unavoided”) crossings in FSSH. Global flux surface hopping (GFSH) generalizes FSSH to treat super-exchange. Second quantized surface hopping (SQUASH) utilizes second quantization and generalizes FSSH to include both super-exchange and decoherence effects. Extended from Hilbert to Liouville space, FSSH and GFSH improve treatment of coherence and Auger-type processes. The key ideas underlying these NAMD-TDDFT approaches will be introduced and illustrated by applications to excited state dynamics in nanoscale materials.

Oleg V. Prezhdo obtained a Diploma in Theoretical Chemistry in 1991 from Kharkiv National University, Ukraine, under Anatoly Luzanov. He completed his Ph.D. with Peter Rossky at the University of Texas, Austin. After a postdoctoral fellowship with John Tully at Yale University, he joined the chemistry department at the University of Washington in 1998, achieving Associate and Full Professor in 2002 and 2005. In 2008, he was elected Fellow of the American Physical Society. In 2010, he was offered a Senior Professorship at the University of Rochester, and in 2014 at the University of Southern California. Since 2008, he has served as editor for the Journal of Physical Chemistry, since 2011 for the Journal of Physical Chemistry Letters, and since 2012 for Progress in Surface Science. Recipient of multiple national and international awards, he held invited professorships in France, Germany, and Japan. His current research interests range from fundamental aspects of semiclassical physics, to excitation dynamics in nano-scale and biological systems.