Published in
Nature Research, Nature Communications, 1(6), 2015
DOI: 10.1038/ncomms7359
Links
- ORCID
- ORCID
- ORCID
- ORCID
- ORCID
- Nature Research | PDF
- [www.ncbi.nlm.nih.gov] | PDF
- [www.researchgate.net] | PDF
- [www.ncbi.nlm.nih.gov] | PDF
- [europepmc.org] | PDF
- [bib-pubdb1.desy.de] | PDF
- [orbit.dtu.dk] | PDF
- [orbit.dtu.dk] | PDF
- [real.mtak.hu] | PDF
- [curis.ku.dk] | PDF
Tools
Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses
,
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
and other authors.
Full text: Download
Abstract
AbstractUltrafast 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.