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      Directing the path of light-induced electron transfer at a molecular fork using vibrational excitation

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          Abstract

          With recent and improved understanding of how nuclear and electronic degrees of freedom can interact with each other comes the opportunity to directly control electronic processes. Now it has been shown that ultrafast vibrational excitation can direct light-induced intramolecular electron transfer along a specific path.

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          Most cited references 44

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          Contemporary Issues in Electron Transfer Research

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            The role of non-equilibrium vibrational structures in electronic coherence and recoherence in pigment–protein complexes

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              Electronic resonance with anticorrelated pigment vibrations drives photosynthetic energy transfer outside the adiabatic framework.

              The delocalized, anticorrelated component of pigment vibrations can drive nonadiabatic electronic energy transfer in photosynthetic light-harvesting antennas. In femtosecond experiments, this energy transfer mechanism leads to excitation of delocalized, anticorrelated vibrational wavepackets on the ground electronic state that exhibit not only 2D spectroscopic signatures attributed to electronic coherence and oscillatory quantum energy transport but also a cross-peak asymmetry not previously explained by theory. A number of antennas have electronic energy gaps matching a pigment vibrational frequency with a small vibrational coordinate change on electronic excitation. Such photosynthetic energy transfer steps resemble molecular internal conversion through a nested intermolecular funnel.
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                Author and article information

                Journal
                Nature Chemistry
                Nature Chem
                Springer Nature
                1755-4330
                1755-4349
                June 19 2017
                June 19 2017
                :
                :
                Article
                10.1038/nchem.2793
                © 2017
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