LEMKE, Henrik T.; KJÆR, Kasper S.; HARTSOCK, Robert; VAN DRIEL, Tim B.; CHOLLET, Matthieu; GLOWNIA, James M.; SANGHOON, Song; ZHU, Diling; PACE, Elisabetta; MATAR, Samir F.; NIELSEN, Martin M.; BENFATTO, Maurizio; GAFFNEY, Kelly J.; COLLET, Eric; CAMMARATA, Marco

doi:10.1038/ncomms15342

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LEMKE, Henrik T.
Paul Scherrer Institute [PSI]

KJÆR, Kasper S.
PULSE Institute
Molecular Movies
Department of Chemical Physics

HARTSOCK, Robert
PULSE Institute

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Article de revue

Ce document a été publié dans

Nature Communications. 2017, vol. 8, n° 1, p. 15342

Nature Publishing Group

Résumé en anglais

The description of ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remains challenging because electronic and nuclear configurations impact each other and cannot be treated independently. Here we gain experimental insights, beyond the Born-Oppenheimer approximation, into the light-induced spin-state trapping dynamics of the prototypical [Fe(bpy)3](2+) compound by time-resolved X-ray absorption spectroscopy at sub-30-femtosecond resolution and high signal-to-noise ratio. The electronic decay from the initial optically excited electronic state towards the high spin state is distinguished from the structural trapping dynamics, which launches a coherent oscillating wave packet (265 fs period), clearly identified as molecular breathing. Throughout the structural trapping, the dispersion of the wave packet along the reaction coordinate reveals details of intramolecular vibronic coupling before a slower vibrational energy dissipation to the solution environment. These findings illustrate how modern time-resolved X-ray absorption spectroscopy can provide key information to unravel dynamic details of photo-functional molecules.< Réduire

DOI

http://dx.doi.org/10.1038/ncomms15342

Project ANR

Etude femtoseconde rayons X et optique de la dynamique ultrarapide de photocommutation de matériaux moléculaires magnétiques

Origine

Importé de hal

Unités de recherche

Institut de Chimie de la Matière Condensée de Bordeaux (ICMCB) - UMR 5026