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

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