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

Biasin, Elisa; Driel, Tim Brandt van; Kjær, Kasper S. LU ; Dohn, Asmus O.; Christensen, Morten; Harlang, Tobias LU ; Chabera, Pavel LU ; Liu, Yizhu LU ; Uhlig, Jens LU and Pápai, Mátyás, et al. (2016) In Phys. Rev. Lett. 117(1).
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... (More)
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. (Less)
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@article{b880f72c-94da-49e0-9461-8b1036ed2bb7,
  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.},
  articleno    = {013002},
  author       = {Biasin, Elisa and Driel, Tim Brandt van and Kjær, Kasper S. and Dohn, Asmus O. and Christensen, Morten and Harlang, Tobias and Chabera, Pavel and Liu, Yizhu and Uhlig, Jens and Pápai, Mátyás and Németh, Zoltán and Hartsock, Robert and Liang, Winnie and Zhang, Jianxin and Alonso-Mori, Roberto and Chollet, Matthieu and Glownia, James M. and Nelson, Silke and Sokaras, Dimosthenis and Assefa, Tadesse A. and Britz, Alexander and Galler, Andreas and Gawelda, Wojciech and Bressler, Christian and Gaffney, Kelly J. and Lemke, Henrik T. and Møller, Klaus B. and Nielsen, Martin M. and Sundström, Villy and Vankó, György and Wärnmark, Kenneth and Canton, Sophie E. and Haldrup, Kristoffer},
  language     = {eng},
  month        = {06},
  number       = {1},
  publisher    = {American Physical Society (APS)},
  series       = {Phys. Rev. Lett.},
  title        = {Femtosecond X-Ray Scattering Study of Ultrafast Photoinduced Structural Dynamics in Solvated[Co(terpy)2]2$},
  url          = {http://dx.doi.org/10.1103/physrevlett.117.013002},
  volume       = {117},
  year         = {2016},
}