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

Elisa Biasin; Tim Brandt van Driel; Kasper S. Kjær; Asmus O. Dohn; Morten Christensen; Tobias Harlang; Pavel Chabera; Yizhu Liu; Jens Uhlig; Mátyás Pápai; Zoltán Németh; Robert Hartsock; Winnie Liang; Jianxin Zhang; Roberto Alonso-Mori; Matthieu Chollet; James M. Glownia; Silke Nelson; Dimosthenis Sokaras; Tadesse A. Assefa; Alexander Britz; Andreas Galler; Wojciech Gawelda; Christian Bressler; Kelly J. Gaffney; Henrik T. Lemke; Klaus B. Møller; Martin M. Nielsen; Villy Sundström; György Vankó; Kenneth Wärnmark; Sophie E. Canton; Kristoffer Haldrup

doi:10.1103/physrevlett.117.013002

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

Elisa Biasin, Tim Brandt van Driel, Kasper S. Kjær, Asmus O. Dohn, Morten Christensen, Tobias Harlang, Pavel Chabera, Yizhu Liu, Jens Uhlig, Mátyás Pápai, Zoltán Németh, Robert Hartsock, Winnie Liang, Jianxin Zhang, Roberto Alonso-Mori, Matthieu Chollet, James M. Glownia, Silke Nelson, Dimosthenis Sokaras, Tadesse A. AssefaAlexander Britz, Andreas Galler, Wojciech Gawelda, Christian Bressler, Kelly J. Gaffney, Henrik T. Lemke, Klaus B. Møller, Martin M. Nielsen, Villy Sundström, György Vankó, Kenneth Wärnmark, Sophie E. Canton, 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 language	English
Article number	013002
Journal	Physical Review Letters
Volume	117
Issue number	1
DOIs	https://doi.org/10.1103/physrevlett.117.013002
Publication status	Published - 2016 Jun 1

Subject classification (UKÄ)

Physical Chemistry
Atom and Molecular Physics and Optics

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10.1103/physrevlett.117.013002

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Biasin, E., Driel, T. B. V., Kjær, K. S., Dohn, A. O., Christensen, M., Harlang, T., Chabera, P., Liu, Y., Uhlig, J., Pápai, M., Németh, Z., Hartsock, R., Liang, W., Zhang, J., Alonso-Mori, R., Chollet, M., Glownia, J. M., Nelson, S., Sokaras, D., ... Haldrup, K. (2016). Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated[Co(terpy)2]2$. Physical Review Letters, 117(1), Article 013002. https://doi.org/10.1103/physrevlett.117.013002

@article{b880f72c94da49e094618b1036ed2bb7,

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 Driel, {Tim Brandt van} and Kj{\ae}r, {Kasper S.} and Dohn, {Asmus O.} and Morten Christensen and Tobias Harlang and Pavel Chabera and Yizhu Liu and Jens Uhlig and M{\'a}ty{\'a}s P{\'a}pai and Zolt{\'a}n N{\'e}meth and Robert Hartsock and Winnie Liang and Jianxin Zhang and Roberto Alonso-Mori and Matthieu Chollet and Glownia, {James M.} and Silke Nelson and Dimosthenis Sokaras and Assefa, {Tadesse A.} and Alexander Britz and Andreas Galler and Wojciech Gawelda and Christian Bressler and Gaffney, {Kelly J.} and Lemke, {Henrik T.} and M{\o}ller, {Klaus B.} and Nielsen, {Martin M.} and Villy Sundstr{\"o}m and Gy{\"o}rgy Vank{\'o} and Kenneth W{\"a}rnmark and Canton, {Sophie E.} and Kristoffer Haldrup",

year = "2016",

month = jun,

day = "1",

doi = "10.1103/physrevlett.117.013002",

language = "English",

volume = "117",

journal = "Physical Review Letters",

issn = "1079-7114",

publisher = "American Physical Society",

number = "1",

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Biasin, E, Driel, TBV, Kjær, KS, Dohn, AO, Christensen, M, Harlang, T, Chabera, P, Liu, Y, Uhlig, J, Pápai, M, Németh, Z, Hartsock, R, Liang, W, Zhang, J, Alonso-Mori, R, Chollet, M, Glownia, JM, Nelson, S, Sokaras, D, Assefa, TA, Britz, A, Galler, A, Gawelda, W, Bressler, C, Gaffney, KJ, Lemke, HT, Møller, KB, Nielsen, MM, Sundström, V, Vankó, G, Wärnmark, K, Canton, SE & Haldrup, K 2016, 'Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated[Co(terpy)2]2$', Physical Review Letters, vol. 117, no. 1, 013002. https://doi.org/10.1103/physrevlett.117.013002

TY - JOUR

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

AU - Biasin, Elisa

AU - Driel, Tim Brandt van

AU - Kjær, Kasper S.

AU - Dohn, Asmus O.

AU - Christensen, Morten

AU - Harlang, Tobias

AU - Chabera, Pavel

AU - Liu, Yizhu

AU - Uhlig, Jens

AU - Pápai, Mátyás

AU - Németh, Zoltán

AU - Hartsock, Robert

AU - Liang, Winnie

AU - Zhang, Jianxin

AU - Alonso-Mori, Roberto

AU - Chollet, Matthieu

AU - Glownia, James M.

AU - Nelson, Silke

AU - Sokaras, Dimosthenis

AU - Assefa, Tadesse A.

AU - Britz, Alexander

AU - Galler, Andreas

AU - Gawelda, Wojciech

AU - Bressler, Christian

AU - Gaffney, Kelly J.

AU - Lemke, Henrik T.

AU - Møller, Klaus B.

AU - Nielsen, Martin M.

AU - Sundström, Villy

AU - Vankó, György

AU - Wärnmark, Kenneth

AU - Canton, Sophie E.

AU - Haldrup, Kristoffer

PY - 2016/6/1

Y1 - 2016/6/1

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.

UR - http://10.1103/PhysRevLett.124.199902

U2 - 10.1103/physrevlett.117.013002

DO - 10.1103/physrevlett.117.013002

M3 - Article

SN - 1079-7114

VL - 117

JO - Physical Review Letters

JF - Physical Review Letters

IS - 1

M1 - 013002

ER -

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

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