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Acetylacetone photodynamics at a seeded free-electron laser

Journal article
Authors Richard J. Squibb
M. Sapunar
A. Ponzi
R. Richter
A. Kivimäki
O. Plekan
P. Finetti
N. Sisourat
Vitali Zhaunerchyk
T. Marchenko
L. Journel
R. Guillemin
R. Cucini
M. Coreno
C. Grazioli
M. Di Fraia
C. Callegari
K.C. Prince
P. Decleva
M. Simon
John H. D. Eland
N. Doslic
Raimund Feifel
M.N. Piancastelli
Published in Nature Communications
Volume 9
ISSN 2041-1723
Publication year 2018
Published at Department of Physics (GU)
Language en
Subject categories Atom and Molecular Physics and Optics, Physical Sciences


Thefirst steps in photochemical processes, such as photosynthesis or animal vision, involvechanges in electronic and geometric structure on extremely short time scales. Time-resolvedphotoelectron spectroscopy is a natural way to measure such changes, but has been hinderedhitherto by limitations of available pulsed light sources in the vacuum-ultraviolet and soft X-ray spectral region, which have insufficient resolution in time and energy simultaneously. Theunique combination of intensity, energy resolution, and femtosecond pulse duration of theFERMI-seeded free-electron laser can now provide exceptionally detailed information onphotoexcitation–deexcitation and fragmentation in pump-probe experiments on the 50-femtosecond time scale. For the prototypical system acetylacetone we report here electronspectra measured as a function of time delay with enough spectral and time resolution tofollow several photoexcited species through well-characterized individual steps, interpretedusing state-of-the-art static and dynamics calculations. These results open the way forinvestigations of photochemical processes in unprecedented detail.

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