Fewest switches surface hopping with Baeck-An couplings.
Computational chemistry
Ethylene
Fewest Switches
Fulvene
Nonadiabatic dynamics
Surface hopping
Ultrafast dynamics
Journal
Open research Europe
ISSN: 2732-5121
Titre abrégé: Open Res Eur
Pays: Belgium
ID NLM: 9918230081006676
Informations de publication
Date de publication:
2021
2021
Historique:
accepted:
01
03
2022
medline:
9
3
2022
pubmed:
9
3
2022
entrez:
30
8
2023
Statut:
epublish
Résumé
In the Baeck-An (BA) approximation, first-order nonadiabatic coupling vectors are given in terms of adiabatic energy gaps and the second derivative of the gaps with respect to the coupling coordinate. In this paper, a time-dependent (TD) BA approximation is derived, where the couplings are computed from the energy gaps and their second time-derivatives. TD-BA couplings can be directly used in fewest switches surface hopping, enabling nonadiabatic dynamics with any electronic structure methods able to provide excitation energies and energy gradients. Test results of surface hopping with TD-BA couplings for ethylene and fulvene show that the TD-BA approximation delivers a qualitatively correct picture of the dynamics and a semiquantitative agreement with reference data computed with exact couplings. Nevertheless, TD-BA does not perform well in situations conjugating strong couplings and small velocities. Considered the uncertainties in the method, TD-BA couplings could be a competitive approach for inexpensive, exploratory dynamics with a small trajectories ensemble. We also assessed the potential use of TD-BA couplings for surface hopping dynamics with time-dependent density functional theory (TDDFT), but the results are not encouraging due to singlet instabilities near the crossing seam with the ground state.
Identifiants
pubmed: 37645211
doi: 10.12688/openreseurope.13624.2
pmc: PMC10446015
doi:
Banques de données
figshare
['10.6084/m9.figshare.14446998.v1']
Types de publication
Journal Article
Langues
eng
Pagination
49Informations de copyright
Copyright: © 2022 T. do Casal M et al.
Déclaration de conflit d'intérêts
No competing interests were disclosed.
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