Communication: GAIMS-Generalized Ab Initio Multiple Spawning for both internal conversion and intersystem crossing processes

Curchod, Basile F.E.; Rauer, Clemens; Marquetand, Philipp; Gonzalez, Leticia; Martinez, Todd J.

doi:10.1063/1.4943571

Communication: GAIMS-Generalized Ab Initio Multiple Spawning for both internal conversion and intersystem crossing processes

Curchod, Basile F.E.; Rauer, Clemens; Marquetand, Philipp; Gonzalez, Leticia; Martinez, Todd J.

Authors

Dr Basile Curchod basile.f.curchod@durham.ac.uk
Academic Visitor

Clemens Rauer

Philipp Marquetand

Leticia Gonzalez

Todd J. Martinez

Abstract

Full multiple spawning is a formally exact method to describe the excited-state dynamics of molecular systems beyond the Born-Oppenheimer approximation. However, it has been limited until now to the description of radiationless transitions taking place between electronic states with the same spin multiplicity. This Communication presents a generalization of the full and ab initio multiple spawning methods to both internal conversion (mediated by nonadiabatic coupling terms) and intersystem crossing events (triggered by spin-orbit coupling matrix elements) based on a spin-diabatic representation. The results of two numerical applications, a model system and the deactivation of thioformaldehyde, validate the presented formalism and its implementation.

Citation

Curchod, B. F., Rauer, C., Marquetand, P., Gonzalez, L., & Martinez, T. J. (2016). Communication: GAIMS-Generalized Ab Initio Multiple Spawning for both internal conversion and intersystem crossing processes. The Journal of Chemical Physics, 144(10), Article 101102. https://doi.org/10.1063/1.4943571

Journal Article Type	Article
Acceptance Date	Feb 26, 2016
Online Publication Date	Mar 11, 2016
Publication Date	Mar 11, 2016
Deposit Date	Nov 6, 2017
Publicly Available Date	Dec 8, 2017
Journal	Journal of Chemical Physics
Print ISSN	0021-9606
Electronic ISSN	1089-7690
Publisher	American Institute of Physics
Peer Reviewed	Peer Reviewed
Volume	144
Issue	10
Article Number	101102
DOI	https://doi.org/10.1063/1.4943571

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© 2016 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in The Journal of Chemical Physics 144, 101102 (2016) and may be found at https://doi.org/10.1063/1.4943571