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

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    Authors
    Delor, Milan cc
    Archer, Stuart A.
    Keane, Theo cc
    Meijer, Anthony J. H. M. cc
    Sazanovich, Igor V.
    Greetham, Gregory M.
    Towrie, Michael
    Weinstein, Julia A. cc
    Affiliation
    University of Sheffield
    Research Complex at Harwell
    Issue Date
    2017-06-19
    
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    Abstract
    Ultrafast electron transfer in condensed-phase molecular systems is often strongly coupled to intramolecular vibrations that can promote, suppress and direct electronic processes. Recent experiments exploring this phenomenon proved that light-induced electron transfer can be strongly modulated by vibrational excitation, suggesting a new avenue for active control over molecular function. Here, we achieve the first example of such explicit vibrational control through judicious design of a Pt(II)-acetylide charge-transfer Donor-Bridge-Acceptor-Bridge-Donor “fork” system: asymmetric 13C isotopic labelling of one of the two -C≡C-bridges makes the two parallel and otherwise identical Donor→Acceptor electron-transfer pathways structurally distinct, enabling independent vibrational perturbation of either. Applying an ultrafast UVpump(excitation)-IRpump(perturbation)-IRprobe(monitoring) pulse sequence, we show that the pathway that is vibrationally perturbed during UV-induced electron-transfer is dramatically slowed down compared to its unperturbed counterpart. One can thus choose the dominant electron transfer pathway. The findings deliver a new opportunity for precise perturbative control of electronic energy propagation in molecular devices.
    Citation
    Delor, M. et al. (2017) ‘Directing the path of light-induced electron transfer at a molecular fork using vibrational excitation’, Nature Chemistry, 9 (11), pp. 1099–1104. doi: 10.1038/nchem.2793
    Publisher
    Springer
    Journal
    Nature Chemistry
    URI
    http://hdl.handle.net/10545/623056
    DOI
    10.1038/nchem.2793
    Additional Links
    http://www.nature.com/doifinder/10.1038/nchem.2793
    Type
    Article
    Language
    en
    ISSN
    1755-4330
    EISSN
    1755-4349
    ae974a485f413a2113503eed53cd6c53
    10.1038/nchem.2793
    Scopus Count
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