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Excited-State Dynamics of Molecules with Classically-Driven Trajectories and Gaussians

Ibele, Lea M.; Nicolson, Angus J.; Curchod, Basile F.E.

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Authors

Lea M. Ibele

Angus J. Nicolson



Abstract

Simulating the dynamics of a molecule initiated in an excited electronic state constitutes a rather challenging task for theoretical and computational chemistry, as such dynamics leads to a strong coupling between nuclear motion and electronic states, that is, a breakdown of the Born–Oppenheimer approximation. This New Views article proposes a brief overview on recent theoretical developments aiming at simulating the excited-state dynamics of molecules – nonadiabatic molecular dynamics – focusing in particular on strategies employing travelling basis functions to portray the dynamics of nuclear wavefunctions. We start by discussing the central equations for nonadiabatic molecular dynamics in a Born–Huang representation. We then propose a comparison between two commonly employed strategies to simulate the excited-state dynamics of molecular systems in their full configuration space, Ab Initio Multiple Spawning (AIMS) and Trajectory Surface Hopping (TSH). The equations of motion for the two techniques are compared and used to contrast their respective description of phenomena involving the decoherence of nuclear wavepackets. Some recent works and developments of the AIMS method are then summarised. This New Views article ends with a highlight on the Exact Factorisation of the molecular wavefunction and how this approach contrasts with the more conventional Born–Huang picture when it comes to the description of photophysical and photochemical processes.

Citation

Ibele, L. M., Nicolson, A. J., & Curchod, B. F. (2020). Excited-State Dynamics of Molecules with Classically-Driven Trajectories and Gaussians. Molecular Physics, 118(8), Article e1665199. https://doi.org/10.1080/00268976.2019.1665199

Journal Article Type Article
Acceptance Date Sep 1, 2019
Online Publication Date Sep 27, 2019
Publication Date 2020
Deposit Date Jun 4, 2019
Publicly Available Date Oct 8, 2019
Journal Molecular Physics
Print ISSN 0026-8976
Electronic ISSN 1362-3028
Publisher Taylor and Francis Group
Peer Reviewed Peer Reviewed
Volume 118
Issue 8
Article Number e1665199
DOI https://doi.org/10.1080/00268976.2019.1665199

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Published Journal Article (Advance online version) (2.6 Mb)
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Publisher Licence URL
http://creativecommons.org/licenses/by/4.0/

Copyright Statement
Advance online version © 2019 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/licenses/by/4.0/), which permits unrestricted use,
distribution, and reproduction in any medium, provided the original work is properly cited.





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