Recent Progress in Surface Hopping: 2011–2015

• Published in: The journal of physical chemistry letters Vol. 7; no. 11; pp. 2100 - 2112
• Main Authors: Wang, Linjun, Akimov, Alexey, Prezhdo, Oleg V
• Format: Journal Article
• Language: English
• Published: United States American Chemical Society 02-06-2016
• Subjects: Quantum Theory; Surface Properties
• ISSN: 1948-7185; 1948-7185
• DOI: 10.1021/acs.jpclett.6b00710

Developed 25 years ago, Tully’s fewest switches surface hopping (FSSH) has proven to be the most popular approach for simulating quantum-classical dynamics in a broad variety of systems, ranging from the gas phase, to the liquid and solid phases, to biological and nanoscale materials. FSSH is widely adopted as the fundamental platform to introduce modifications as needed. Significant progress has been made recently to enhance the accuracy and efficiency of the surface hopping technique. Various limitations of the standard FSSHassociated with quantum nuclear effects, interference and decoherence, trivial or “unavoided” crossings, superexchange, and representation dependencehave been lifted. These advances are needed to allow one to treat many important phenomena in chemistry, physics, materials, and related disciplines. Examples include charge transport in extended systems such as organic solids, singlet fission in molecular aggregates, Auger-type exciton multiplication, recombination and relaxation in quantum dots and other nanoscale materials, Auger-assisted charge transfer, nonradiative luminescence quenching, and electron–hole recombination. This Perspective summarizes recent advances in the surface hopping formulation of nonadiabatic dynamics and provides an outlook on the future of surface hopping.