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Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule

Haldrup, Kristoffer; Levi, Gianluca; Biasin, Elisa; Vester, Peter; Laursen, Mads Goldschmidt; Beyer, Frederik; Kjær, Kasper Skov LU ; Brandt Van Driel, Tim; Harlang, Tobias LU and Dohn, Asmus O., et al. (2019) In Physical Review Letters 122(6).
Abstract

We report x-ray free electron laser experiments addressing ground-state structural dynamics of the diplatinum anion Pt2POP4 following photoexcitation. The structural dynamics are tracked with <100 fs time resolution by x-ray scattering, utilizing the anisotropic component to suppress contributions from the bulk solvent. The x-ray data exhibit a strong oscillatory component with period 0.28 ps and decay time 2.2 ps, and structural analysis of the difference signal directly shows this as arising from ground-state dynamics along the PtPt coordinate. These results are compared with multiscale Born-Oppenheimer molecular dynamics simulations and demonstrate how off-resonance excitation can be used to prepare a vibrationally cold... (More)

We report x-ray free electron laser experiments addressing ground-state structural dynamics of the diplatinum anion Pt2POP4 following photoexcitation. The structural dynamics are tracked with <100 fs time resolution by x-ray scattering, utilizing the anisotropic component to suppress contributions from the bulk solvent. The x-ray data exhibit a strong oscillatory component with period 0.28 ps and decay time 2.2 ps, and structural analysis of the difference signal directly shows this as arising from ground-state dynamics along the PtPt coordinate. These results are compared with multiscale Born-Oppenheimer molecular dynamics simulations and demonstrate how off-resonance excitation can be used to prepare a vibrationally cold excited-state population complemented by a structure-dependent depletion of the ground-state population which subsequently evolves in time, allowing direct tracking of ground-state structural dynamics.

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Physical Review Letters
volume
122
issue
6
publisher
American Physical Society
external identifiers
  • scopus:85061555095
ISSN
0031-9007
DOI
10.1103/PhysRevLett.122.063001
language
English
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yes
id
d22ff347-8b71-4719-b3a9-3141cb4146eb
date added to LUP
2019-02-21 11:03:17
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2019-04-23 04:46:08
@article{d22ff347-8b71-4719-b3a9-3141cb4146eb,
  abstract     = {<p>We report x-ray free electron laser experiments addressing ground-state structural dynamics of the diplatinum anion Pt2POP4 following photoexcitation. The structural dynamics are tracked with &lt;100 fs time resolution by x-ray scattering, utilizing the anisotropic component to suppress contributions from the bulk solvent. The x-ray data exhibit a strong oscillatory component with period 0.28 ps and decay time 2.2 ps, and structural analysis of the difference signal directly shows this as arising from ground-state dynamics along the PtPt coordinate. These results are compared with multiscale Born-Oppenheimer molecular dynamics simulations and demonstrate how off-resonance excitation can be used to prepare a vibrationally cold excited-state population complemented by a structure-dependent depletion of the ground-state population which subsequently evolves in time, allowing direct tracking of ground-state structural dynamics.</p>},
  articleno    = {063001},
  author       = {Haldrup, Kristoffer and Levi, Gianluca and Biasin, Elisa and Vester, Peter and Laursen, Mads Goldschmidt and Beyer, Frederik and Kjær, Kasper Skov and Brandt Van Driel, Tim and Harlang, Tobias and Dohn, Asmus O. and Hartsock, Robert J. and Nelson, Silke and Glownia, James M. and Lemke, Henrik T. and Christensen, Morten and Gaffney, Kelly J. and Henriksen, Niels E. and Møller, Klaus B. and Nielsen, Martin M.},
  issn         = {0031-9007},
  language     = {eng},
  month        = {02},
  number       = {6},
  publisher    = {American Physical Society},
  series       = {Physical Review Letters},
  title        = {Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule},
  url          = {http://dx.doi.org/10.1103/PhysRevLett.122.063001},
  volume       = {122},
  year         = {2019},
}