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

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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.


  • Kristoffer Haldrup
  • Gianluca Levi
  • Elisa Biasin
  • Peter Vester
  • Mads Goldschmidt Laursen
  • Frederik Beyer
  • Kasper Skov Kjær
  • Tim Brandt Van Driel
  • Tobias Harlang
  • Asmus O. Dohn
  • Robert J. Hartsock
  • Silke Nelson
  • James M. Glownia
  • Henrik T. Lemke
  • Morten Christensen
  • Kelly J. Gaffney
  • Niels E. Henriksen
  • Klaus B. Møller
  • Martin M. Nielsen
Enheter & grupper
Externa organisationer
  • Technical University of Denmark
  • University of Iceland
  • SLAC National Accelerator Laboratory
  • Paul Scherrer Institute

Ämnesklassifikation (UKÄ) – OBLIGATORISK

  • Atom- och molekylfysik och optik
TidskriftPhysical Review Letters
Utgåva nummer6
StatusPublished - 2019 feb 13
Peer review utfördJa