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  Toward a Correct Description of Initial Electronic Coherence in Nonadiabatic Dynamics Simulations

Mannouch, J., & Kelly, A. (2024). Toward a Correct Description of Initial Electronic Coherence in Nonadiabatic Dynamics Simulations. The Journal of Physical Chemistry Letters, 15(46), 11687-11695. doi:10.1021/acs.jpclett.4c02418.

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mannouch-kelly-2024-toward-a-correct-description-of-initial-electronic-coherence-in-nonadiabatic-dynamics-simulations.pdf (Publisher version), 4MB
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https://arxiv.org/abs/2408.09547 (Preprint)
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https://doi.org/10.1021/acs.jpclett.4c02418 (Publisher version)
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 Creators:
Mannouch, J.1, 2, Author           
Kelly, A.1, 2, Author           
Affiliations:
1Hamburg Center for Ultrafast Imaging, Universität Hamburg, ou_persistent22              
2Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              

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 Abstract: The recent improvement in experimental capabilities for interrogating and controlling molecular systems with ultrafast coherent light sources calls for the development of theoretical approaches that can accurately and efficiently treat electronic coherence. However, the most popular and practical nonadiabatic molecular dynamics techniques, Tully’s fewest-switches surface hopping and Ehrenfest mean-field dynamics, are unable to describe the dynamics proceeding from an initial electronic coherence. While such issues are not encountered with the analogous coupled-trajectory algorithms or numerically exact quantum dynamics methods, applying such techniques necessarily comes with a higher computational cost. Here we show that a correct description of initial electronic coherence can indeed be achieved using independent-trajectory methods derived from the semiclassical mapping formalism. The key is the introduction of an initial sampling over the electronic phase space and a means of incorporating phase interference between trajectories, both of which are naturally achieved when working within the semiclassical mapping framework.

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Language(s): eng - English
 Dates: 2024-11-082024-08-182024-11-112024-11-14
 Publication Status: Published online
 Pages: 9
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 Table of Contents: -
 Rev. Type: Peer
 Identifiers: arXiv: 2408.09547
DOI: 10.1021/acs.jpclett.4c02418
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Project name : This work was supported by the Cluster of Excellence “CUI: Advanced Imaging of Matter” of the Deutsche Forschungsgemeinschaft (DFG) (EXC 2056, Project 390715994). J.R.M. also acknowledges support from the Alexander von Humboldt Foundation.
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Title: The Journal of Physical Chemistry Letters
  Abbreviation : J. Phys. Chem. Lett.
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: - Volume / Issue: 15 (46) Sequence Number: - Start / End Page: 11687 - 11695 Identifier: ISSN: 1948-7185
CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185