Journal article
Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule
Department of Physics, Technical University of Denmark1
Neutrons and X-rays for Materials Physics, Department of Physics, Technical University of Denmark2
Department of Chemistry, Technical University of Denmark3
Department of Chemical and Biochemical Engineering, Technical University of Denmark4
The Danish Polymer Centre, Department of Chemical and Biochemical Engineering, Technical University of Denmark5
SLAC National Accelerator Laboratory6
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.
Language: | English |
---|---|
Year: | 2019 |
Pages: | 063001 |
ISSN: | 10797114 and 00319007 |
Types: | Journal article |
DOI: | 10.1103/PhysRevLett.122.063001 |
ORCIDs: | Haldrup, Kristoffer , Biasin, Elisa , Vester, Peter , Kjær, Kasper Skov , Dohn, Asmus O. , Henriksen, Niels E. , Møller, Klaus B. and Nielsen, Martin M. |