Journal
NATURE COMMUNICATIONS
Volume 6, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms7359
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Funding
- X-ray Free-Electron Laser Priority Strategy Program of MEXT,Japan
- Swedish Research Council
- Knut and Alice Wallenberg Foundation
- Crafoord Foundation
- Swedish Energy Administration
- Science Faculty at Lund University (MAXIV)
- Science Faculty at Lund University (ESS initiative grant)
- Danish National Research Foundation Center for Molecular Movies
- DANSCATT
- Carlsberg Foundation
- Lundbeck Foundation
- European Research Council [ERC-AdvGVISCHEM-226136, ERC-StG-259709]
- European XFEL
- German Research Foundation (DFG) [SFB925]
- Centre of Ultrafast Imaging (CUI)
- Hungarian Academy of Sciences via the Lendulet (Momentum) Program
- Bolyai Fellowship
- US Department of Energy, Office of Science, Office of Basic Energy Sciences [DE-AC02-06CH11357]
- Grants-in-Aid for Scientific Research [26102014] Funding Source: KAKEN
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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.
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