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

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

*Corresponding author for this work

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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.

Original languageEnglish
Article number063001
JournalPhysical Review Letters
Issue number6
Number of pages8
Publication statusPublished - 2019

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