SSAIMS - Stochastic-Selection Ab Initio Multiple Spawning for Efficient Nonadiabatic Molecular Dynamics

Curchod, Basile F.E.; Glover, W.J.; Martinez, T.J.

doi:10.1021/acs.jpca.0c04113

SSAIMS - Stochastic-Selection Ab Initio Multiple Spawning for Efficient Nonadiabatic Molecular Dynamics

Curchod, Basile F.E.; Glover, W.J.; Martinez, T.J.

Authors

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

W.J. Glover

T.J. Martinez

Abstract

Ab initio multiple spawning provides a powerful and accurate way of describing the excited-state dynamics of molecular systems, whose strength resides in the proper description of coherence effects during nonadiabatic processes thanks to the coupling of trajectory basis functions. However, the simultaneous propagation of a large number of trajectory basis functions can be numerically inconvenient. We propose here an elegant and simple solution to this issue, which consists of (i) detecting uncoupled groups of coupled trajectory basis functions, and (ii) selecting stochastically one of these groups to continue the AIMS dynamics. We show that this procedure can reproduce the results of full AIMS dynamics in cases where the uncoupled groups of TBFs stay uncoupled throughout the dynamics (which is often the case in high dimensional problems). We present and discuss the aforementioned idea in detail and provide simple numerical applications on indole, ethylene and protonated formaldimine, highlighting the potential of stochastic-selection ab initio multiple spawning.

Citation

Curchod, B. F., Glover, W., & Martinez, T. (2020). SSAIMS - Stochastic-Selection Ab Initio Multiple Spawning for Efficient Nonadiabatic Molecular Dynamics. The Journal of Physical Chemistry A, 124(30), 6133-6143. https://doi.org/10.1021/acs.jpca.0c04113

Journal Article Type	Article
Acceptance Date	Jun 25, 2020
Online Publication Date	Jul 30, 2020
Publication Date	Jul 31, 2020
Deposit Date	Jun 25, 2020
Publicly Available Date	Jul 30, 2020
Journal	The Journal of Physical Chemistry A
Print ISSN	1089-5639
Electronic ISSN	1520-5215
Publisher	American Chemical Society
Peer Reviewed	Peer Reviewed
Volume	124
Issue	30
Pages	6133-6143
DOI	https://doi.org/10.1021/acs.jpca.0c04113

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