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Title: Anisotropy enhanced X-ray scattering from solvated transition metal complexes

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 photoexcitation of a solvated di-platinum complex at an XFEL, and the key parameters involved are explored. Here 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 responsemore » function.« less

Authors:
 [1];  [2];  [3];  [4];  [5];  [4];  [4];  [4];  [6];  [4];  [7];  [4];  [7];  [3];  [3];  [4];  [4]
  1. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
  2. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States). Linac Coherent Light Source (LCLS)
  3. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Chemistry
  4. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics
  5. Univ. of Iceland, Reykjavík (Iceland). Faculty of Physical Sciences
  6. Technical Univ. of Denmark, Lyngby (Denmark). Dept. of Physics; SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE); Lund Univ. (Sweden). Dept. of Chemical Physics
  7. SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); Danish Council for Independent Research (DFF)
OSTI Identifier:
1427028
Grant/Contract Number:  
AC02-76SF00515; DFF 4002-00272B
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Synchrotron Radiation (Online)
Additional Journal Information:
Journal Name: Journal of Synchrotron Radiation (Online); Journal Volume: 25; Journal Issue: 2; Journal ID: ISSN 1600-5775
Publisher:
International Union of Crystallography
Country of Publication:
United States
Language:
English
Subject:
71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS; time-resolved; anisotropic scattering; orientational selection; XFEL; ultrafast; molecular structure

Citation Formats

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., Harlang, Tobias, Hartsock, Robert, Christensen, Morten, Gaffney, Kelly J., Henriksen, Niels E., Møller, Klaus B., Haldrup, Kristoffer, and Nielsen, Martin M.. Anisotropy enhanced X-ray scattering from solvated transition metal complexes. United States: N. p., 2018. Web. doi:10.1107/s1600577517016964.
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., Harlang, Tobias, Hartsock, Robert, Christensen, Morten, Gaffney, Kelly J., Henriksen, Niels E., Møller, Klaus B., Haldrup, Kristoffer, & Nielsen, Martin M.. Anisotropy enhanced X-ray scattering from solvated transition metal complexes. United States. doi:10.1107/s1600577517016964.
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., Harlang, Tobias, Hartsock, Robert, Christensen, Morten, Gaffney, Kelly J., Henriksen, Niels E., Møller, Klaus B., Haldrup, Kristoffer, and Nielsen, Martin M.. Tue . "Anisotropy enhanced X-ray scattering from solvated transition metal complexes". United States. doi:10.1107/s1600577517016964.
@article{osti_1427028,
title = {Anisotropy enhanced X-ray scattering from solvated transition metal complexes},
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.},
abstractNote = {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. Here 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.},
doi = {10.1107/s1600577517016964},
journal = {Journal of Synchrotron Radiation (Online)},
number = 2,
volume = 25,
place = {United States},
year = {Tue Feb 13 00:00:00 EST 2018},
month = {Tue Feb 13 00:00:00 EST 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on February 13, 2019
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