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Anisotropy enhanced X-ray scattering from solvated transition metal complexes

Biasin, Elisa ; Van Driel, Tim B. ; Levi, Gianluca ; Laursen, Mads G. ; Dohn, Asmus O. ; Moltke, Asbjørn ; Vester, Peter ; Hansen, Frederik B.K. ; Kjaer, Kasper S. LU and Harlang, Tobias LU , et al. (2018) In Journal of Synchrotron Radiation 25(2). p.306-315
Abstract

Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV-Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolved X-ray scattering patterns measured upon... (More)

Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV-Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolved X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. It is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute, i.e. the change in Pt - Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.The analysis of time-resolved X-ray scattering patterns collected at an XFEL upon photoexcitation of a di-platinum complex in solution is described. The analysis quantitatively considers the anisotropy of the signal.

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organization
publishing date
type
Contribution to journal
publication status
published
subject
keywords
anisotropic scattering, molecular structure, orientational selection, time-resolved, ultrafast, XFEL
in
Journal of Synchrotron Radiation
volume
25
issue
2
pages
10 pages
publisher
International Union of Crystallography
external identifiers
  • scopus:85042688943
  • pmid:29488907
ISSN
0909-0495
DOI
10.1107/S1600577517016964
language
English
LU publication?
yes
id
dfe53b94-a355-40b8-a220-9399d3c363e2
date added to LUP
2018-03-19 10:45:49
date last changed
2024-06-11 12:30:25
@article{dfe53b94-a355-40b8-a220-9399d3c363e2,
  abstract     = {{<p>Time-resolved X-ray scattering patterns from photoexcited molecules in solution are in many cases anisotropic at the ultrafast time scales accessible at X-ray free-electron lasers (XFELs). This anisotropy arises from the interaction of a linearly polarized UV-Vis pump laser pulse with the sample, which induces anisotropic structural changes that can be captured by femtosecond X-ray pulses. In this work, a method for quantitative analysis of the anisotropic scattering signal arising from an ensemble of molecules is described, and it is demonstrated how its use can enhance the structural sensitivity of the time-resolved X-ray scattering experiment. This method is applied on time-resolved X-ray scattering patterns measured upon photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. It is shown that a combined analysis of the anisotropic and isotropic difference scattering signals in this experiment allows a more precise determination of the main photoinduced structural change in the solute, i.e. the change in Pt - Pt bond length, and yields more information on the excitation channels than the analysis of the isotropic scattering only. Finally, it is discussed how the anisotropic transient response of the solvent can enable the determination of key experimental parameters such as the instrument response function.The analysis of time-resolved X-ray scattering patterns collected at an XFEL upon photoexcitation of a di-platinum complex in solution is described. The analysis quantitatively considers the anisotropy of the signal.</p>}},
  author       = {{Biasin, Elisa and Van Driel, Tim B. and Levi, Gianluca and Laursen, Mads G. and Dohn, Asmus O. and Moltke, Asbjørn and Vester, Peter and Hansen, Frederik B.K. and Kjaer, Kasper S. and Harlang, Tobias and Hartsock, Robert and Christensen, Morten and Gaffney, Kelly J. and Henriksen, Niels E. and Møller, Klaus B. and Haldrup, Kristoffer and Nielsen, Martin M.}},
  issn         = {{0909-0495}},
  keywords     = {{anisotropic scattering; molecular structure; orientational selection; time-resolved; ultrafast; XFEL}},
  language     = {{eng}},
  month        = {{03}},
  number       = {{2}},
  pages        = {{306--315}},
  publisher    = {{International Union of Crystallography}},
  series       = {{Journal of Synchrotron Radiation}},
  title        = {{Anisotropy enhanced X-ray scattering from solvated transition metal complexes}},
  url          = {{http://dx.doi.org/10.1107/S1600577517016964}},
  doi          = {{10.1107/S1600577517016964}},
  volume       = {{25}},
  year         = {{2018}},
}