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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching.

hal.structure.identifierPaul Scherrer Institute [PSI]
dc.contributor.authorLEMKE, Henrik T.
hal.structure.identifierPULSE Institute
hal.structure.identifierMolecular Movies
hal.structure.identifierDepartment of Chemical Physics
dc.contributor.authorKJÆR, Kasper S.
hal.structure.identifierPULSE Institute
dc.contributor.authorHARTSOCK, Robert
hal.structure.identifierMolecular Movies
dc.contributor.authorVAN DRIEL, Tim B.
dc.contributor.authorCHOLLET, Matthieu
dc.contributor.authorGLOWNIA, James M.
dc.contributor.authorSANGHOON, Song
dc.contributor.authorZHU, Diling
hal.structure.identifierLaboratori Nazionali di Frascati
dc.contributor.authorPACE, Elisabetta
hal.structure.identifierInstitut de Chimie de la Matière Condensée de Bordeaux [ICMCB]
dc.contributor.authorMATAR, Samir F.
hal.structure.identifierMolecular Movies
dc.contributor.authorNIELSEN, Martin M.
hal.structure.identifierLaboratori Nazionali di Frascati
dc.contributor.authorBENFATTO, Maurizio
hal.structure.identifierPULSE Institute
hal.structure.identifierStanford Synchrotron Radiation Lightsource [SSRL SLAC]
dc.contributor.authorGAFFNEY, Kelly J.
hal.structure.identifierInstitut de Physique de Rennes [IPR]
dc.contributor.authorCOLLET, Eric
hal.structure.identifierInstitut de Physique de Rennes [IPR]
dc.contributor.authorCAMMARATA, Marco
dc.date.issued2017
dc.identifier.issn2041-1723
dc.description.abstractEnThe 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.sponsorshipEtude femtoseconde rayons X et optique de la dynamique ultrarapide de photocommutation de matériaux moléculaires magnétiques
dc.language.isoen
dc.publisherNature Publishing Group
dc.title.enCoherent structural trapping through wave packet dispersion during photoinduced spin state switching.
dc.typeArticle de revue
dc.identifier.doi10.1038/ncomms15342
dc.subject.halChimie/Chimie de coordination
dc.subject.halChimie/Chimie théorique et/ou physique
dc.subject.halPhysique [physics]
bordeaux.journalNature Communications
bordeaux.page15342
bordeaux.volume8
bordeaux.issue1
bordeaux.peerReviewedoui
hal.identifierhal-01538614
hal.version1
hal.popularnon
hal.audienceInternationale
hal.origin.linkhttps://hal.archives-ouvertes.fr//hal-01538614v1
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