Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+

Elisa Biasin, Tim Brandt van Driel, Kasper Skov Kjær, Asmus Ougaard Dohn, Morten Christensen, Tobias Harlang, Pavel Chabera, Yizhu Liu, Jens Uhlig, Mátyás Imre Pápai, Klaus Braagaard Møller, Martin Meedom Nielsen, Kristoffer Haldrup

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Abstract

We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ∼7 ps.
Original languageEnglish
Article number013002
JournalPhysical Review Letters
Volume117
Issue number1
Number of pages6
ISSN0031-9007
DOIs
Publication statusPublished - 2016

Cite this

Biasin, Elisa ; Brandt van Driel, Tim ; Kjær, Kasper Skov ; Dohn, Asmus Ougaard ; Christensen, Morten ; Harlang, Tobias ; Chabera, Pavel ; Liu, Yizhu ; Uhlig, Jens ; Pápai, Mátyás Imre ; Møller, Klaus Braagaard ; Nielsen, Martin Meedom ; Haldrup, Kristoffer. / Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+. In: Physical Review Letters. 2016 ; Vol. 117, No. 1.
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title = "Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+",
abstract = "We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ∼7 ps.",
author = "Elisa Biasin and {Brandt van Driel}, Tim and Kj{\ae}r, {Kasper Skov} and Dohn, {Asmus Ougaard} and Morten Christensen and Tobias Harlang and Pavel Chabera and Yizhu Liu and Jens Uhlig and P{\'a}pai, {M{\'a}ty{\'a}s Imre} and M{\o}ller, {Klaus Braagaard} and Nielsen, {Martin Meedom} and Kristoffer Haldrup",
year = "2016",
doi = "10.1103/PhysRevLett.117.013002",
language = "English",
volume = "117",
journal = "Physical Review Letters",
issn = "0031-9007",
publisher = "American Physical Society",
number = "1",

}

Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+. / Biasin, Elisa; Brandt van Driel, Tim; Kjær, Kasper Skov; Dohn, Asmus Ougaard; Christensen, Morten; Harlang, Tobias; Chabera, Pavel; Liu, Yizhu; Uhlig, Jens; Pápai, Mátyás Imre; Møller, Klaus Braagaard; Nielsen, Martin Meedom; Haldrup, Kristoffer.

In: Physical Review Letters, Vol. 117, No. 1, 013002, 2016.

Research output: Contribution to journalJournal articleResearchpeer-review

TY - JOUR

T1 - Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated [Co(terpy)2]2+

AU - Biasin, Elisa

AU - Brandt van Driel, Tim

AU - Kjær, Kasper Skov

AU - Dohn, Asmus Ougaard

AU - Christensen, Morten

AU - Harlang, Tobias

AU - Chabera, Pavel

AU - Liu, Yizhu

AU - Uhlig, Jens

AU - Pápai, Mátyás Imre

AU - Møller, Klaus Braagaard

AU - Nielsen, Martin Meedom

AU - Haldrup, Kristoffer

PY - 2016

Y1 - 2016

N2 - We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ∼7 ps.

AB - We study the structural dynamics of photoexcited [Co(terpy)2]2+ in an aqueous solution with ultrafast x-ray diffuse scattering experiments conducted at the Linac Coherent Light Source. Through direct comparisons with density functional theory calculations, our analysis shows that the photoexcitation event leads to elongation of the Co-N bonds, followed by coherent Co-N bond length oscillations arising from the impulsive excitation of a vibrational mode dominated by the symmetrical stretch of all six Co-N bonds. This mode has a period of 0.33 ps and decays on a subpicosecond time scale. We find that the equilibrium bond-elongated structure of the high spin state is established on a single-picosecond time scale and that this state has a lifetime of ∼7 ps.

U2 - 10.1103/PhysRevLett.117.013002

DO - 10.1103/PhysRevLett.117.013002

M3 - Journal article

C2 - 27419566

VL - 117

JO - Physical Review Letters

JF - Physical Review Letters

SN - 0031-9007

IS - 1

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