Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated
Abstract
Here, 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.
- Authors:
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- Technical Univ. of Denmark, Lyngby (Denmark)
- Technical Univ. of Denmark, Lyngby (Denmark); Lund Univ., Lund (Sweden); SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Lund Univ., Lund (Sweden)
- Technical Univ. of Denmark, Lyngby (Denmark): Hungarian Academy Sciences, Budapest (Hungary)
- Hungarian Academy Sciences, Budapest (Hungary)
- SLAC National Accelerator Lab., Menlo Park, CA (United States)
- Tianjin Polytechnic Univ., Tianjin (China)
- European XFEL GmbH, Hamburg (Germany)
- European XFEL GmbH, Hamburg (Germany); Jan Kochanowski Univ., Kielce (Poland)
- SLAC National Accelerator Lab., Menlo Park, CA (United States); Paul Scherrer Inst. (PSI), Villigen (Switzerland)
- Max Planck Institute for Biophysical Chemistry, Goettingen (Germany); Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
- Publication Date:
- Research Org.:
- SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1335954
- Alternate Identifier(s):
- OSTI ID: 1259990
- Grant/Contract Number:
- StG-259709; K29724; LP2013-59; 21302138; AC02-76SF00515; 20130504
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Letters
- Additional Journal Information:
- Journal Volume: 117; Journal Issue: 1; Journal ID: ISSN 0031-9007
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 43 PARTICLE ACCELERATORS
Citation Formats
Biasin, Elisa, van Driel, Tim Brandt, Kjær, Kasper S., Dohn, Asmus O., Christensen, Morten, Harlang, Tobias, Chabera, Pavel, Liu, Yizhu, Uhlig, Jens, Papai, Matyas, Nemeth, Zoltan, Hartsock, Robert, Liang, Winnie, Zhang, Jianxin, Alonso-Mori, Roberto, Chollet, Matthieu, Glownia, James M., Nelson, Silke, Sokaras, Dimosthenis, Assefa, Tadesse A., Britz, Alexander, Galler, Andreas, Gawelda, Wojciech, Bressler, Christian, Gaffney, Kelly J., Lemke, Henrik T., Moller, Klaus B., Nielsen, Martin M., Sundstrom, Villy, Vanko, Gyorgy, Warnmark, Kenneth, Canton, Sophie E., and Haldrup, Kristoffer. Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [Co(terpy)2]2+. United States: N. p., 2016.
Web. doi:10.1103/PhysRevLett.117.013002.
Biasin, Elisa, van Driel, Tim Brandt, Kjær, Kasper S., Dohn, Asmus O., Christensen, Morten, Harlang, Tobias, Chabera, Pavel, Liu, Yizhu, Uhlig, Jens, Papai, Matyas, Nemeth, Zoltan, Hartsock, Robert, Liang, Winnie, Zhang, Jianxin, Alonso-Mori, Roberto, Chollet, Matthieu, Glownia, James M., Nelson, Silke, Sokaras, Dimosthenis, Assefa, Tadesse A., Britz, Alexander, Galler, Andreas, Gawelda, Wojciech, Bressler, Christian, Gaffney, Kelly J., Lemke, Henrik T., Moller, Klaus B., Nielsen, Martin M., Sundstrom, Villy, Vanko, Gyorgy, Warnmark, Kenneth, Canton, Sophie E., & Haldrup, Kristoffer. Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [Co(terpy)2]2+. United States. https://doi.org/10.1103/PhysRevLett.117.013002
Biasin, Elisa, van Driel, Tim Brandt, Kjær, Kasper S., Dohn, Asmus O., Christensen, Morten, Harlang, Tobias, Chabera, Pavel, Liu, Yizhu, Uhlig, Jens, Papai, Matyas, Nemeth, Zoltan, Hartsock, Robert, Liang, Winnie, Zhang, Jianxin, Alonso-Mori, Roberto, Chollet, Matthieu, Glownia, James M., Nelson, Silke, Sokaras, Dimosthenis, Assefa, Tadesse A., Britz, Alexander, Galler, Andreas, Gawelda, Wojciech, Bressler, Christian, Gaffney, Kelly J., Lemke, Henrik T., Moller, Klaus B., Nielsen, Martin M., Sundstrom, Villy, Vanko, Gyorgy, Warnmark, Kenneth, Canton, Sophie E., and Haldrup, Kristoffer. Thu .
"Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [Co(terpy)2]2+". United States. https://doi.org/10.1103/PhysRevLett.117.013002. https://www.osti.gov/servlets/purl/1335954.
@article{osti_1335954,
title = {Femtosecond x-ray scattering study of ultrafast photoinduced structural dynamics in solvated [Co(terpy)2]2+},
author = {Biasin, Elisa and van Driel, Tim Brandt and Kjær, Kasper S. and Dohn, Asmus O. and Christensen, Morten and Harlang, Tobias and Chabera, Pavel and Liu, Yizhu and Uhlig, Jens and Papai, Matyas and Nemeth, Zoltan 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 Moller, Klaus B. and Nielsen, Martin M. and Sundstrom, Villy and Vanko, Gyorgy and Warnmark, Kenneth and Canton, Sophie E. and Haldrup, Kristoffer},
abstractNote = {Here, 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.},
doi = {10.1103/PhysRevLett.117.013002},
journal = {Physical Review Letters},
number = 1,
volume = 117,
place = {United States},
year = {Thu Jun 30 00:00:00 EDT 2016},
month = {Thu Jun 30 00:00:00 EDT 2016}
}
Web of Science
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