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Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses.


ABSTRACT: Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor-acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined.

SUBMITTER: Canton SE 

PROVIDER: S-EPMC4366532 | biostudies-literature | 2015 Mar

REPOSITORIES: biostudies-literature

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Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses.

Canton Sophie E SE   Kjær Kasper S KS   Vankó György G   van Driel Tim B TB   Adachi Shin-ichi S   Bordage Amélie A   Bressler Christian C   Chabera Pavel P   Christensen Morten M   Dohn Asmus O AO   Galler Andreas A   Gawelda Wojciech W   Gosztola David D   Haldrup Kristoffer K   Harlang Tobias T   Liu Yizhu Y   Møller Klaus B KB   Németh Zoltán Z   Nozawa Shunsuke S   Pápai Mátyás M   Sato Tokushi T   Sato Takahiro T   Suarez-Alcantara Karina K   Togashi Tadashi T   Tono Kensuke K   Uhlig Jens J   Vithanage Dimali A DA   Wärnmark Kenneth K   Yabashi Makina M   Zhang Jianxin J   Sundström Villy V   Nielsen Martin M MM  

Nature communications 20150302


Ultrafast photoinduced electron transfer preceding energy equilibration still poses many experimental and conceptual challenges to the optimization of photoconversion since an atomic-scale description has so far been beyond reach. Here we combine femtosecond transient optical absorption spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor-acceptor compl  ...[more]

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