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

Sophie E. Canton (), Kasper S. Kjær (), György Vankó, Tim B. van Driel, Shin-ichi Adachi, Amélie Bordage, Christian Bressler, Pavel Chabera, Morten Christensen, Asmus O. Dohn, Andreas Galler, Wojciech Gawelda, David Gosztola, Kristoffer Haldrup, Tobias Harlang, Yizhu Liu, Klaus B. Møller, Zoltán Németh, Shunsuke Nozawa, Mátyás Pápai, Tokushi Sato, Takahiro Sato, Karina Suarez-Alcantara, Tadashi Togashi, Kensuke Tono, Jens Uhlig, Dimali A. Vithanage, Kenneth Wärnmark, Makina Yabashi, Jianxin Zhang, Villy Sundström and Martin M. Nielsen ()
Additional contact information
Sophie E. Canton: Lund University
Kasper S. Kjær: Centre for Molecular Movies, Niels Bohr Institute, University of Copenhagen
György Vankó: Wigner Research Centre for Physics, Hungarian Academy Sciences
Tim B. van Driel: Centre for Molecular Movies, Technical University of Denmark
Shin-ichi Adachi: High Energy Accelerator Research Organization
Amélie Bordage: Wigner Research Centre for Physics, Hungarian Academy Sciences
Christian Bressler: European XFEL
Pavel Chabera: Lund University
Morten Christensen: Centre for Molecular Movies, Technical University of Denmark
Asmus O. Dohn: Technical University of Denmark
Andreas Galler: European XFEL
Wojciech Gawelda: European XFEL
David Gosztola: Center for Nanoscale Materials, Argonne National Laboratory
Kristoffer Haldrup: Centre for Molecular Movies, Technical University of Denmark
Tobias Harlang: Lund University
Yizhu Liu: Centre for Analysis and Synthesis, Lund University
Klaus B. Møller: Technical University of Denmark
Zoltán Németh: Wigner Research Centre for Physics, Hungarian Academy Sciences
Shunsuke Nozawa: High Energy Accelerator Research Organization
Mátyás Pápai: Wigner Research Centre for Physics, Hungarian Academy Sciences
Tokushi Sato: High Energy Accelerator Research Organization
Takahiro Sato: RIKEN SPring-8 Center
Karina Suarez-Alcantara: Lund University
Tadashi Togashi: Japan Synchrotron Radiation Research Institute (JASRI)
Kensuke Tono: Japan Synchrotron Radiation Research Institute (JASRI)
Jens Uhlig: Lund University
Dimali A. Vithanage: Lund University
Kenneth Wärnmark: Centre for Analysis and Synthesis, Lund University
Makina Yabashi: RIKEN SPring-8 Center
Jianxin Zhang: Centre for Analysis and Synthesis, Lund University
Villy Sundström: Lund University
Martin M. Nielsen: Centre for Molecular Movies, Technical University of Denmark

Nature Communications, 2015, vol. 6, issue 1, 1-10

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms7359

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