Coherent structural trapping through wave packet dispersion during photoinduced spin state switching.
hal.structure.identifier | Paul Scherrer Institute [PSI] | |
dc.contributor.author | LEMKE, Henrik T. | |
hal.structure.identifier | PULSE Institute | |
hal.structure.identifier | Molecular Movies | |
hal.structure.identifier | Department of Chemical Physics | |
dc.contributor.author | KJÆR, Kasper S. | |
hal.structure.identifier | PULSE Institute | |
dc.contributor.author | HARTSOCK, Robert | |
hal.structure.identifier | Molecular Movies | |
dc.contributor.author | VAN DRIEL, Tim B. | |
dc.contributor.author | CHOLLET, Matthieu | |
dc.contributor.author | GLOWNIA, James M. | |
dc.contributor.author | SANGHOON, Song | |
dc.contributor.author | ZHU, Diling | |
hal.structure.identifier | Laboratori Nazionali di Frascati | |
dc.contributor.author | PACE, Elisabetta | |
hal.structure.identifier | Institut de Chimie de la Matière Condensée de Bordeaux [ICMCB] | |
dc.contributor.author | MATAR, Samir F. | |
hal.structure.identifier | Molecular Movies | |
dc.contributor.author | NIELSEN, Martin M. | |
hal.structure.identifier | Laboratori Nazionali di Frascati | |
dc.contributor.author | BENFATTO, Maurizio | |
hal.structure.identifier | PULSE Institute | |
hal.structure.identifier | Stanford Synchrotron Radiation Lightsource [SSRL SLAC] | |
dc.contributor.author | GAFFNEY, Kelly J. | |
hal.structure.identifier | Institut de Physique de Rennes [IPR] | |
dc.contributor.author | COLLET, Eric | |
hal.structure.identifier | Institut de Physique de Rennes [IPR] | |
dc.contributor.author | CAMMARATA, Marco | |
dc.date.issued | 2017 | |
dc.identifier.issn | 2041-1723 | |
dc.description.abstractEn | 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. | |
dc.description.sponsorship | Etude femtoseconde rayons X et optique de la dynamique ultrarapide de photocommutation de matériaux moléculaires magnétiques | |
dc.language.iso | en | |
dc.publisher | Nature Publishing Group | |
dc.title.en | Coherent structural trapping through wave packet dispersion during photoinduced spin state switching. | |
dc.type | Article de revue | |
dc.identifier.doi | 10.1038/ncomms15342 | |
dc.subject.hal | Chimie/Chimie de coordination | |
dc.subject.hal | Chimie/Chimie théorique et/ou physique | |
dc.subject.hal | Physique [physics] | |
bordeaux.journal | Nature Communications | |
bordeaux.page | 15342 | |
bordeaux.volume | 8 | |
bordeaux.issue | 1 | |
bordeaux.peerReviewed | oui | |
hal.identifier | hal-01538614 | |
hal.version | 1 | |
hal.popular | non | |
hal.audience | Internationale | |
hal.origin.link | https://hal.archives-ouvertes.fr//hal-01538614v1 | |
bordeaux.COinS | ctx_ver=Z39.88-2004&rft_val_fmt=info:ofi/fmt:kev:mtx:journal&rft.jtitle=Nature%20Communications&rft.date=2017&rft.volume=8&rft.issue=1&rft.spage=15342&rft.epage=15342&rft.eissn=2041-1723&rft.issn=2041-1723&rft.au=LEMKE,%20Henrik%20T.&KJ%C3%86R,%20Kasper%20S.&HARTSOCK,%20Robert&VAN%20DRIEL,%20Tim%20B.&CHOLLET,%20Matthieu&rft.genre=article |
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