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

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@article{17d5a233fe1a438498b9f9038943033b,
title = "Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule",
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 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.",
author = "Kristoffer Haldrup and Gianluca Levi and Elisa Biasin and Peter Vester and Laursen, {Mads Goldschmidt} and Frederik Beyer and Kj{\ae}r, {Kasper Skov} and {Brandt Van Driel}, Tim and Tobias Harlang and Dohn, {Asmus O.} and Hartsock, {Robert J.} and Silke Nelson and Glownia, {James M.} and Lemke, {Henrik T.} and Morten Christensen and Gaffney, {Kelly J.} and Henriksen, {Niels E.} and M{\o}ller, {Klaus B.} and Nielsen, {Martin M.}",
year = "2019",
doi = "10.1103/PhysRevLett.122.063001",
language = "English",
volume = "122",
journal = "Physical Review Letters",
issn = "0031-9007",
publisher = "American Physical Society",
number = "6",

}

RIS

TY - JOUR

T1 - Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule

AU - Haldrup, Kristoffer

AU - Levi, Gianluca

AU - Biasin, Elisa

AU - Vester, Peter

AU - Laursen, Mads Goldschmidt

AU - Beyer, Frederik

AU - Kjær, Kasper Skov

AU - Brandt Van Driel, Tim

AU - Harlang, Tobias

AU - Dohn, Asmus O.

AU - Hartsock, Robert J.

AU - Nelson, Silke

AU - Glownia, James M.

AU - Lemke, Henrik T.

AU - Christensen, Morten

AU - Gaffney, Kelly J.

AU - Henriksen, Niels E.

AU - Møller, Klaus B.

AU - Nielsen, Martin M.

PY - 2019

Y1 - 2019

N2 - 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.

AB - 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.

U2 - 10.1103/PhysRevLett.122.063001

DO - 10.1103/PhysRevLett.122.063001

M3 - Journal article

VL - 122

JO - Physical Review Letters

JF - Physical Review Letters

SN - 0031-9007

IS - 6

M1 - 063001

ER -