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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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.

Original languageEnglish
Article number063001
JournalPhysical Review Letters
Volume122
Issue number6
Number of pages8
ISSN0031-9007
DOIs
Publication statusPublished - 2019

Cite this

Haldrup, Kristoffer ; Levi, Gianluca ; Biasin, Elisa ; Vester, Peter ; Laursen, Mads Goldschmidt ; Beyer, Frederik ; Kjær, Kasper Skov ; Brandt Van Driel, Tim ; Harlang, Tobias ; Dohn, Asmus O. ; Hartsock, Robert J. ; Nelson, Silke ; Glownia, James M. ; Lemke, Henrik T. ; Christensen, Morten ; Gaffney, Kelly J. ; Henriksen, Niels E. ; Møller, Klaus B. ; Nielsen, Martin M. / Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule. In: Physical Review Letters. 2019 ; Vol. 122, No. 6.
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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",

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Haldrup, K, Levi, G, Biasin, E, Vester, P, Laursen, MG, Beyer, F, Kjær, KS, Brandt Van Driel, T, Harlang, T, Dohn, AO, Hartsock, RJ, Nelson, S, Glownia, JM, Lemke, HT, Christensen, M, Gaffney, KJ, Henriksen, NE, Møller, KB & Nielsen, MM 2019, 'Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule', Physical Review Letters, vol. 122, no. 6, 063001. https://doi.org/10.1103/PhysRevLett.122.063001

Ultrafast X-Ray Scattering Measurements of Coherent Structural Dynamics on the Ground-State Potential Energy Surface of a Diplatinum Molecule. / Haldrup, Kristoffer; Levi, Gianluca; Biasin, Elisa; Vester, Peter; Laursen, Mads Goldschmidt; Beyer, Frederik; Kjær, Kasper Skov; Brandt Van Driel, Tim; Harlang, Tobias; Dohn, Asmus O.; Hartsock, Robert J.; Nelson, Silke; Glownia, James M.; Lemke, Henrik T.; Christensen, Morten; Gaffney, Kelly J.; Henriksen, Niels E.; Møller, Klaus B.; Nielsen, Martin M.

In: Physical Review Letters, Vol. 122, No. 6, 063001, 2019.

Research output: Contribution to journalJournal articleResearchpeer-review

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 -