Journal
NATURE COMMUNICATIONS
Volume 9, Issue -, Pages -Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/s41467-017-02478-0
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Funding
- Knut and Alice Wallenberg Foundation, Sweden
- Swedish Research Council
- UKF
- Croatian Science Foundation [IP-2016-06-1142]
- Italian-Slovenian Crossborder Cooperation Programme (CITIUS project) [2013/2010090600115298]
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The first steps in photochemical processes, such as photosynthesis or animal vision, involve changes in electronic and geometric structure on extremely short time scales. Time-resolved photoelectron spectroscopy is a natural way to measure such changes, but has been hindered hitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft Xray spectral region, which have insufficient resolution in time and energy simultaneously. The unique combination of intensity, energy resolution, and femtosecond pulse duration of the FERMI-seeded free-electron laser can now provide exceptionally detailed information on photoexcitation-deexcitation and fragmentation in pump-probe experiments on the 50-femtosecond time scale. For the prototypical system acetylacetone we report here electron spectra measured as a function of time delay with enough spectral and time resolution to follow several photoexcited species through well-characterized individual steps, interpreted using state-of-the-art static and dynamics calculations. These results open the way for investigations of photochemical processes in unprecedented detail.
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