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  Excited-State Vibronic Dynamics of Bacteriorhodopsin from Two-Dimensional Electronic Photon Echo Spectroscopy and Multiconfigurational Quantum Chemistry

Gozem, S., Johnson, P. J. M., Halpin, A., Luk, H. L., Morizumi, T., Prokhorenko, V., et al. (2020). Excited-State Vibronic Dynamics of Bacteriorhodopsin from Two-Dimensional Electronic Photon Echo Spectroscopy and Multiconfigurational Quantum Chemistry. The Journal of Physical Chemistry Letters, 11(10), 3889-3896. doi:10.1021/acs.jpclett.0c01063.

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Item Permalink: http://hdl.handle.net/21.11116/0000-0006-8FE1-B Version Permalink: http://hdl.handle.net/21.11116/0000-0006-8FE2-A
Genre: Journal Article

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https://dx.doi.org/10.1021/acs.jpclett.0c01063 (Publisher version)
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 Creators:
Gozem, S.1, Author
Johnson, P. J. M.2, Author
Halpin, A.2, Author
Luk, H. L.1, Author
Morizumi, T.3, Author
Prokhorenko, V.4, Author              
Ernst, O. P.5, Author
Olivucci, M.1, Author
Miller, R. J. D.2, Author
Affiliations:
1Department of Chemistry, Bowling Green State University, ou_persistent22              
2Department of Chemistry and Department of Physics, University of Toronto, ou_persistent22              
3Department of Biochemistry, University of Toronto, ou_persistent22              
4Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
5Department of Biochemistry and Department of Molecular Genetics, University of Toronto, ou_persistent22              

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 Abstract: Owing to the ultrafast time scale of the photoinduced reaction and high degree of spectral overlap among the reactant, product, and excited electronic states in bacteriorhodopsin (bR), it has been a challenge for traditional spectroscopies to resolve the interplay between vibrational dynamics and electronic processes occurring in the retinal chromophore of bR. Here, we employ ultrafast two-dimensional electronic photon echo spectroscopy to follow the early excited-state dynamics of bR preceding the isomerization. We detect an early periodic photoinduced absorptive signal that, employing a hybrid multiconfigurational quantum/molecular mechanical model of bR, we attribute to periodic mixing of the first and second electronic excited states (S1 and S2, respectively). This recurrent interaction between S1 and S2, induced by a bond length alternation of the retinal chromohore, supports the hypothesis that the ultrafast photoisomerization in bR is initiated by a process involving coupled nuclear and electronic motion on three different electronic states.

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Language(s): eng - English
 Dates: 2020-04-042020-04-242020-04-242020-05-21
 Publication Status: Published in print
 Pages: 8
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 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.jpclett.0c01063
 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: 11 (10) Sequence Number: - Start / End Page: 3889 - 3896 Identifier: CoNE: https://pure.mpg.de/cone/journals/resource/1948-7185