The Ehrenfest method with fully quantum nuclear motion (Qu-Eh): application to charge migration in radical cations
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Published version
Author(s)
Jenkins, Andrew J
Spinlove, Kaite
Vacher, Morgane
Worth, Graham A
Robb, MA
Type
Journal Article
Abstract
An algorithm is described for quantum dynamics where an Ehrenfest potential is combined with fully quantum nuclear motion (Quantum-Ehrenfest, Qu-Eh). The method is related to the single-set variational multi-configuration Gaussian approach (vMCG) but has the advantage that only a single quantum chemistry computation is required at each time step since there is only a single time-dependent potential surface. Also shown is the close relationship to the “exact factorization method.” The quantum Ehrenfest method is compared with vMCG for study of electron dynamics in a modified bismethylene-adamantane cation system. Illustrative examples of electron-nuclear dynamics are presented for a distorted allene system and for HCCI+ where one has a degenerate Π system.
Date Issued
2018-09-07
Date Acceptance
2018-08-21
Citation
Journal of Chemical Physics, 2018, 149 (9)
ISSN
0021-9606
Publisher
AIP Publishing
Journal / Book Title
Journal of Chemical Physics
Volume
149
Issue
9
Copyright Statement
© 2018 Author(s). All article content, except where otherwise noted, is licensed under a Creative Commons Attribution (CC BY) license (http://creativecommons.org/licenses/by/4.0/)
Subjects
Science & Technology
Physical Sciences
Chemistry, Physical
Physics, Atomic, Molecular & Chemical
Chemistry
Physics
CONFIGURATION GAUSSIAN WAVEPACKETS
MOLECULAR-DYNAMICS
ELECTRON
IMPLEMENTATION
IONIZATION
02 Physical Sciences
03 Chemical Sciences
09 Engineering
Chemical Physics
Publication Status
Published
Article Number
094108
Date Publish Online
2018-09-07