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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
by
van Driel, Tim B.
, Chollet, Matthieu
, Hartsock, Robert
, Nielsen, Martin M.
, Kjær, Kasper S.
, Cammarata, Marco
, Benfatto, Maurizio
, Pace, Elisabetta
, Glownia, James M.
, Matar, Samir F.
, Collet, Eric
, Zhu, Diling
, Gaffney, Kelly J.
, Song, Sanghoon
, Lemke, Henrik T.
in
140/125
/ 639/624/1111
/ 639/638/439
/ 639/766/94
/ Absorption spectroscopy
/ Approximation
/ Atom and Molecular Physics and Optics
/ Atom- och molekylfysik och optik (Här ingår: Kemisk fysik, kvantoptik)
/ ATOMIC AND MOLECULAR PHYSICS
/ Chemical Sciences
/ Coordination chemistry
/ Energy dissipation
/ Fysik
/ Humanities and Social Sciences
/ Ligands
/ multidisciplinary
/ Natural Sciences
/ Naturvetenskap
/ or physical chemistry
/ Physical Sciences
/ Physics
/ Science
/ Science (multidisciplinary)
/ Spectrum analysis
/ Theoretical and
/ Trapping
/ Vibration
2017
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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
by
van Driel, Tim B.
, Chollet, Matthieu
, Hartsock, Robert
, Nielsen, Martin M.
, Kjær, Kasper S.
, Cammarata, Marco
, Benfatto, Maurizio
, Pace, Elisabetta
, Glownia, James M.
, Matar, Samir F.
, Collet, Eric
, Zhu, Diling
, Gaffney, Kelly J.
, Song, Sanghoon
, Lemke, Henrik T.
in
140/125
/ 639/624/1111
/ 639/638/439
/ 639/766/94
/ Absorption spectroscopy
/ Approximation
/ Atom and Molecular Physics and Optics
/ Atom- och molekylfysik och optik (Här ingår: Kemisk fysik, kvantoptik)
/ ATOMIC AND MOLECULAR PHYSICS
/ Chemical Sciences
/ Coordination chemistry
/ Energy dissipation
/ Fysik
/ Humanities and Social Sciences
/ Ligands
/ multidisciplinary
/ Natural Sciences
/ Naturvetenskap
/ or physical chemistry
/ Physical Sciences
/ Physics
/ Science
/ Science (multidisciplinary)
/ Spectrum analysis
/ Theoretical and
/ Trapping
/ Vibration
2017
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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
by
van Driel, Tim B.
, Chollet, Matthieu
, Hartsock, Robert
, Nielsen, Martin M.
, Kjær, Kasper S.
, Cammarata, Marco
, Benfatto, Maurizio
, Pace, Elisabetta
, Glownia, James M.
, Matar, Samir F.
, Collet, Eric
, Zhu, Diling
, Gaffney, Kelly J.
, Song, Sanghoon
, Lemke, Henrik T.
in
140/125
/ 639/624/1111
/ 639/638/439
/ 639/766/94
/ Absorption spectroscopy
/ Approximation
/ Atom and Molecular Physics and Optics
/ Atom- och molekylfysik och optik (Här ingår: Kemisk fysik, kvantoptik)
/ ATOMIC AND MOLECULAR PHYSICS
/ Chemical Sciences
/ Coordination chemistry
/ Energy dissipation
/ Fysik
/ Humanities and Social Sciences
/ Ligands
/ multidisciplinary
/ Natural Sciences
/ Naturvetenskap
/ or physical chemistry
/ Physical Sciences
/ Physics
/ Science
/ Science (multidisciplinary)
/ Spectrum analysis
/ Theoretical and
/ Trapping
/ Vibration
2017
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Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
Journal Article
Coherent structural trapping through wave packet dispersion during photoinduced spin state switching
2017
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Overview
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.
Ultrafast nonadiabatic chemical dynamics during molecular photo-transformations remain challenging to describe since electronic/nuclear configurations are coupled. Here the authors use time-resolved X-ray absorption spectroscopy to probe the light-induced spin-state trapping dynamics of [Fe(bpy)
3
]
2+
beyond the Born-Oppenheimer approximation.
Publisher
Nature Publishing Group UK,Nature Publishing Group,Nature Portfolio
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