Journal article
Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses
Lund University1
The Hamburg Centre for Ultrafast Imaging2
European XFEL3
Argonne National Laboratory4
RIKEN5
Japan Synchrotron Radiation Research Institute6
University of Copenhagen7
Hungarian Academy of Sciences8
Department of Physics, Technical University of Denmark9
Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark10
Center for Atomic-scale Materials Design, Centers, Technical University of Denmark11
Department of Chemistry, Technical University of Denmark12
Physical and Biophysical Chemistry, Department of Chemistry, Technical University of Denmark13
High Energy Accelerator Research Organization14
...and 4 moreUltrafast 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.
Language: | English |
---|---|
Publisher: | Nature Pub. Group |
Year: | 2015 |
Pages: | 6359 |
ISSN: | 20411723 |
Types: | Journal article |
DOI: | 10.1038/ncomms7359 |
ORCIDs: | 0000-0002-2472-1684 , Dohn, Asmus Ougaard , Haldrup, Kristoffer , Møller, Klaus Braagaard and Nielsen, Martin Meedom |