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

Canton, Sophie LU ; Kjær, Kasper S; Vankó, György; van Driel, Tim B; Adachi, Shin-Ichi; Bordage, Amélie; Bressler, Christian; Chabera, Pavel; Christensen, Morten and Dohn, Asmus O, et al. (2015) In Nature Communications 6.
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... (More)
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. (Less)
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Nature Communications
volume
6
publisher
Nature Publishing Group
external identifiers
  • pmid:25727920
  • wos:000352719000001
  • scopus:84923876685
ISSN
2041-1723
DOI
10.1038/ncomms7359
language
English
LU publication?
yes
id
28f69a28-b84e-4c96-be7b-0461f7ddaa52 (old id 5265607)
date added to LUP
2015-04-10 15:23:11
date last changed
2017-11-19 03:56:46
@article{28f69a28-b84e-4c96-be7b-0461f7ddaa52,
  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.},
  articleno    = {6359},
  author       = {Canton, Sophie and Kjær, Kasper S and Vankó, György and van Driel, Tim B and Adachi, Shin-Ichi and Bordage, Amélie and Bressler, Christian and Chabera, Pavel and Christensen, Morten and Dohn, Asmus O and Galler, Andreas and Gawelda, Wojciech and Gosztola, David and Haldrup, Kristoffer and Harlang, Tobias and Liu, Yizhu and Møller, Klaus B and Németh, Zoltán and Nozawa, Shunsuke and Pápai, Mátyás and Sato, Tokushi and Sato, Takahiro and Suarez Alcantara, Karina and Togashi, Tadashi and Tono, Kensuke and Uhlig, Jens and Vithanage, Dimali A and Wärnmark, Kenneth and Yabashi, Makina and Zhang, Jianxin and Sundström, Villy and Nielsen, Martin M},
  issn         = {2041-1723},
  language     = {eng},
  publisher    = {Nature Publishing Group},
  series       = {Nature Communications},
  title        = {Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses.},
  url          = {http://dx.doi.org/10.1038/ncomms7359},
  volume       = {6},
  year         = {2015},
}