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  The Primary Photochemistry of Vision Occurs at the Molecular Speed Limit

Johnson, P. J. M., Farag, M., Halpin, A., Morizumi, T., Prokhorenko, V., Knoester, J., et al. (2017). The Primary Photochemistry of Vision Occurs at the Molecular Speed Limit. The Journal of Physical Chemistry B, 121(16), 4040-4047. doi:10.1021/acs.jpcb.7b02329.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-002D-5A6C-2 Version Permalink: http://hdl.handle.net/21.11116/0000-0001-EAEF-B
Genre: Journal Article

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https://dx.doi.org/10.1021/acs.jpcb.7b02329 (Publisher version)
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 Creators:
Johnson, Philip J. M.1, Author
Farag, Marwa2, 3, Author              
Halpin, Alexei1, Author
Morizumi, Takefumi4, Author
Prokhorenko, Valentyn2, Author              
Knoester, Jasper3, Author
Jansen, Thomas L. C.3, Author
Ernst, Oliver P.4, 5, Author
Miller, R. J. Dwayne1, 2, Author              
Affiliations:
1Departments of Chemistry & Physics, University of Toronto, 80 St. George Street, Toronto, Ontario M5S 3H6, Canada, ou_persistent22              
2Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
3Zernike Institute for Advanced Materials, University of Groningen, Nijenborgh 4, 9747 AG Groningen, The Netherlands, ou_persistent22              
4Department of Biochemistry, University of Toronto, 1 King’s College Circle, Toronto, Ontario M5S 1A8, Canada, ou_persistent22              
5Department of Molecular Genetics, University of Toronto, 1 King’s College Circle, Toronto, Ontario M5S 1A8, Canada, ou_persistent22              

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 Abstract: Ultrafast photochemical reactions are initiated by vibronic transitions from the reactant ground state to the excited potential energy surface, directly populating excited-state vibrational modes. The primary photochemical reaction of vision, the isomerization of retinal in the protein rhodopsin, is known to be a vibrationally coherent reaction, but the Franck–Condon factors responsible for initiating the process have been difficult to resolve with conventional time-resolved spectroscopies. Here we employ experimental and theoretical 2D photon echo spectroscopy to directly resolve for the first time the Franck–Condon factors that initiate isomerization on the excited potential energy surface and track the reaction dynamics. The spectral dynamics reveal vibrationally coherent isomerization occurring on the fastest possible time scale, that of a single period of the local torsional reaction coordinate. We successfully model this process as coherent wavepacket motion through a conical intersection on a ∼30 fs time scale, confirming the reaction coordinate as a local torsional coordinate with a frequency of ∼570 cm–1. As a result of spectral features being spread out along two frequency coordinates, we unambiguously assign reactant and product states following passage through the conical intersection, which reveal the key vibronic transitions that initiate the vibrationally coherent photochemistry of vision.

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Language(s): eng - English
 Dates: 2017-03-292017-03-112017-03-302017-04-27
 Publication Status: Published in print
 Pages: 8
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1021/acs.jpcb.7b02329
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Title: The Journal of Physical Chemistry B
  Abbreviation : J. Phys. Chem. B
Source Genre: Journal
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Publ. Info: Washington, D.C. : American Chemical Society
Pages: - Volume / Issue: 121 (16) Sequence Number: - Start / End Page: 4040 - 4047 Identifier: ISSN: 1520-6106
CoNE: /journals/resource/1000000000293370_1