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  Local vibrational coherences drive the primary photochemistry of vision

Johnson, P. J. M., Halpin, A., Morizumi, T., Prokhorenko, V., Ernst, O. P., & Miller, R. J. D. (2015). Local vibrational coherences drive the primary photochemistry of vision. Nature Chemistry, 7(12), 980-986. doi:10.1038/nchem.2398.

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Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0029-0462-E Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0029-20D1-5
Genre: Journal Article

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http://dx.doi.org/10.1038/nchem.2398 (Publisher version)
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 Creators:
Johnson, Philip J. M.1, Author
Halpin, Alexei1, Author
Morizumi, Takefumi2, Author
Prokhorenko, Valentyn3, Author              
Ernst, Oliver P.2, 4, Author
Miller, R. J. Dwayne1, 3, Author              
Affiliations:
1Institute for Optical Sciences and Departments of Chemistry and Physics, University of Toronto, 80 St George Street, Toronto, Ontario M5S 3H6, Canada, ou_persistent22              
2Department of Biochemistry, University of Toronto, 1 King's College Circle, Toronto, Ontario M5S 1A8, Canada, ou_persistent22              
3Miller Group, Atomically Resolved Dynamics Department, Max Planck Institute for the Structure and Dynamics of Matter, Max Planck Society, ou_1938288              
4Department of Molecular Genetics, University of Toronto, 1 King's College Circle, Toronto, Ontario M5S 1A8, Canada, ou_persistent22              

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Free keywords: Excited states; Reaction kinetics and dynamics; Photobiology; Optical spectroscopy
 Abstract: The role of vibrational coherence—concerted vibrational motion on the excited-state potential energy surface—in the isomerization of retinal in the protein rhodopsin remains elusive, despite considerable experimental and theoretical efforts. We revisited this problem with resonant ultrafast heterodyne-detected transient-grating spectroscopy. The enhanced sensitivity that this technique provides allows us to probe directly the primary photochemical reaction of vision with sufficient temporal and spectral resolution to resolve all the relevant nuclear dynamics of the retinal chromophore during isomerization. We observed coherent photoproduct formation on a sub-50 fs timescale, and recovered a host of vibrational modes of the retinal chromophore that modulate the transient-grating signal during the isomerization reaction. Through Fourier filtering and subsequent time-domain analysis of the transient vibrational dynamics, the excited-state nuclear motions that drive the isomerization reaction were identified, and comprise stretching, torsional and out-of-plane wagging motions about the local C11=C12 isomerization coordinate.

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Language(s): eng - English
 Dates: 2015-04-172015-10-152015-11-162015-12
 Publication Status: Published in print
 Pages: 7
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1038/nchem.2398
 Degree: -

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Title: Nature Chemistry
  Abbreviation : Nat. Chem.
Source Genre: Journal
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Publ. Info: London, UK : Nature Publishing Group
Pages: - Volume / Issue: 7 (12) Sequence Number: - Start / End Page: 980 - 986 Identifier: ISSN: 1755-4330
CoNE: /journals/resource/1755-4330