Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule
(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.
(Less)
- author
- organization
- publishing date
- 2019-02-13
- type
- Contribution to journal
- publication status
- published
- subject
- in
- Physical Review Letters
- volume
- 122
- issue
- 6
- article number
- 063001
- publisher
- American Physical Society
- external identifiers
-
- scopus:85061555095
- pmid:30822093
- ISSN
- 0031-9007
- DOI
- 10.1103/PhysRevLett.122.063001
- language
- English
- LU publication?
- yes
- id
- d22ff347-8b71-4719-b3a9-3141cb4146eb
- date added to LUP
- 2019-02-21 11:03:17
- date last changed
- 2024-09-03 13:17:23
@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 <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>}}, 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}}, doi = {{10.1103/PhysRevLett.122.063001}}, volume = {{122}}, year = {{2019}}, }