Journal
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
Volume 11, Issue 10, Pages 3889-3896Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpclett.0c01063
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Funding
- Natural Sciences and Engineering Research Council of Canada
- Max Planck Society
- Canada Excellence Research Chairs program
- Human Frontier Science Program Organization [RGP0049/2012CHE09-56776]
- Institute for Advanced Studies of the University of Strasbourg
- NSF [CHE-CLP-1710191]
- NIH [1R15GM126627 01]
- MIUR, Dipartimento di Eccellenza
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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 (S-1 and S-2, respectively). This recurrent interaction between S-1 and S-2, 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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