Spin-Mapping Methods for Simulating Ultrafast Nonadiabatic Dynamics
| Autor: | Johan E. Runeson, Jonathan R. Mannouch, Graziano Amati, Marit R. Fiechter, Jeremy O. Richardson |
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| Jazyk: | German<br />English<br />French |
| Rok vydání: | 2022 |
| Předmět: | |
| Zdroj: | CHIMIA, Vol 76, Iss 6 (2022) |
| Druh dokumentu: | article |
| ISSN: | 0009-4293 2673-2424 |
| DOI: | 10.2533/chimia.2022.582 |
| Popis: | 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. |
| Databáze: | Directory of Open Access Journals |
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