A general method to describe intersystem crossing dynamics in trajectory surface hopping

By S. Mai, Philipp Marquetand, L. González. 2015

257 citations recorded by the source corpus.

Intersystem crossing is a radiationless process that can take place in a molecule irradiated by UV-Vis light, thereby playing an important role in many environmental, biological and technological processes. This paper reviews different methods to describe intersystem crossing dynamics, paying attention to semiclassical trajectory theories, which are especially interesting because they can be applied to large systems with many degrees of freedom. In particular, a general trajectory surface hopping methodology recently developed by the authors, which is able to include nonadiabatic and spin-orbit couplings in excited-state dynamics simulations, is explained in detail. This method, termed SHARC, can in principle include any arbitrary coupling, what makes it generally applicable to photophysical and photochemical problems, also those including explicit laser fields. A step-by-step derivation of the main equations of motion employed in surface hopping based on the fewest-switches method of Tully, adapted for the inclusion of spin-orbit interactions, is provided. Special emphasis is put on describing the different possible choices of the electronic bases in which spin-orbit can be included in surface hopping, highlighting the advantages and inconsistencies of the different approaches. © 2015 Wiley Periodicals, Inc.

Subfields: Atomic and Molecular Physics, and Optics, Physical and Theoretical Chemistry

View Paper: https://www.semanticscholar.org/paper/e4771ff99560c0f2bf91a21ce35ca64d19ff4090

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In Atomic and Molecular Physics, and Optics

1. Qijing Zheng
2. Weibin Chu
3. Chuanyu Zhao
4. Lili Zhang
5. Yanan Wang
6. Xiang Jiang
7. Jin Zhao
8. Hongli Guo

Citations in the corpus

• Ab initio nonadiabatic molecular dynamics investigations on the excited carriers in condensed matter systems (2019, methodology): “There are two representation for the SOC included NAMD: the spin diabatic and spin adiabatic representations.(154) In the spin diabatic representation, the spinpolarized KS orbitals are used as basis sets and the SOC contribute to the off-diagonal elements in the Hamiltonian, which determines the pr”