TY - JOUR AU - Runeson, Johan E. AU - Mannouch, Jonathan R. AU - Amati, Graziano AU - Fiechter, Marit R. AU - Richardson, Jeremy O. PY - 2022/06/29 Y2 - 2024/03/29 TI - Spin-Mapping Methods for Simulating Ultrafast Nonadiabatic Dynamics JF - CHIMIA JA - Chimia VL - 76 IS - 6 SE - Scientific Articles DO - 10.2533/chimia.2022.582 UR - https://www.chimia.ch/chimia/article/view/2022_582 SP - 582-588 AB - <p>Many chemical reactions exhibit nonadiabatic effects as a consequence of coupling between electronic states and/or interaction with light. While a fully quantum description of nonadiabatic reactions is unfeasible for most realistic molecules, a more computationally tractable approach is to combine a classical description of the nuclei with a quantum description of the electronic states. Combining the formalisms of quantum and classical dynamics is however a difficult problem for which standard methods (such as Ehrenfest dynamics and surface hopping) may be insufficient. In this article, we review a new trajectory-based approach developed in our group that is able to describe nonadiabatic dynamics with a higher accuracy than previous approaches but for a similar level of computational effort. This method treats the electronic states with a phase-space representation for discrete-level systems, which in the two-level case is analogous to a spin-½. We point out the key features of the method and demonstrate its use in a variety of applications, including ultrafast transfer through conical intersections, damped coherent excitation under coupling to a strong light field, and nonlinear spectroscopy of light-harvesting complexes.</p> ER -