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  Simulating Vibronic Spectra without Born–Oppenheimer Surfaces

Lively, K., Albareda Piquer, G., Sato, S., Kelly, A., & Rubio, A. (2021). Simulating Vibronic Spectra without Born–Oppenheimer Surfaces. The Journal of Physical Chemistry Letters, 12(12), 3074-3081. doi:10.1021/acs.jpclett.1c00073.

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Supporting Information: Details on MTEF, STEF, and ICWF as referenced in the main text
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https://dx.doi.org/10.1021/acs.jpclett.1c00073 (Publisher version)
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https://arxiv.org/abs/2101.03007 (Preprint)
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 Creators:
Lively, K.1, 2, Author              
Albareda Piquer, G.1, 2, 3, 4, Author              
Sato, S.1, 2, 5, Author              
Kelly, A.1, 2, 6, Author              
Rubio, A.1, 2, 4, 7, Author              
Affiliations:
1Theory Group, Theory Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_2266715              
2Center for Free-Electron Laser Science, ou_persistent22              
3Institute of Theoretical and Computational Chemistry, University of Barcelona, ou_persistent22              
4Nano-Bio Spectroscopy Group and ETSF, Universidad del País Vasco, ou_persistent22              
5Center for Computational Sciences, University of Tsukuba, ou_persistent22              
6Department of Chemistry, Dalhousie University, ou_persistent22              
7Center for Computational Quantum Physics (CCQ), Flatiron Institute, ou_persistent22              

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Free keywords: Wave function, Equilibrium, Mathematical methods, Hamiltonians, Computational chemistry
 Abstract: We show how linear vibronic spectra in molecular systems can be simulated efficiently using first-principles approaches without relying on the explicit use of multiple Born–Oppenheimer potential energy surfaces. We demonstrate and analyze the performance of mean-field and beyond-mean-field dynamics techniques for the H2 molecule in one dimension, in the later case capturing the vibronic structure quite accurately, including quantum Franck–Condon effects. In a practical application of this methodology we simulate the absorption spectrum of benzene in full dimensionality using time-dependent density functional theory at the multitrajectory Ehrenfest level, finding good qualitative agreement with experiment and significant spectral reweighting compared to commonly used single-trajectory Ehrenfest dynamics. These results form the foundation for nonlinear spectral calculations and show promise for future application in capturing phenomena associated with vibronic coupling in more complex molecular and potentially condensed phase systems.

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Language(s): eng - English
 Dates: 2021-01-082021-03-152021-03-222021-04-01
 Publication Status: Published in print
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acs.jpclett.1c00073
arXiv: 2101.03007
 Degree: -

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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: 12 (12) Sequence Number: - Start / End Page: 3074 - 3081 Identifier: ISSN: 1948-7185
CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185