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Title: Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure

Abstract

During X-ray exposure of a molecular solution, photons scattered from the same molecule are correlated. If molecular motion is insignificant during exposure, then differences in momentum transfer between correlated photons are direct measurements of the molecular structure. In conventional small- and wide-angle solution scattering, photon correlations are ignored. This report presents advances in a new biomolecular structural analysis technique, correlated X-ray scattering (CXS), which uses angular intensity correlations to recover hidden structural details from molecules in solution. Due to its intense rapid pulses, an X-ray free electron laser (XFEL) is an excellent tool for CXS experiments. A protocol is outlined for analysis of a CXS data set comprising a total of half a million X-ray exposures of solutions of small gold nanoparticles recorded at the Spring-8 Ångström Compact XFEL facility (SACLA). From the scattered intensities and their correlations, two populations of nanoparticle domains within the solution are distinguished: small twinned, and large probably non-twinned domains. Finally, it is shown analytically how, in a solution measurement, twinning information is only accessible via intensity correlations, demonstrating how CXS reveals atomic-level information from a disordered solution of like molecules.

Authors:
 [1];  [1];  [1];  [1];  [2];  [1];  [3];  [3];  [4];  [4];  [5];  [2];  [6]
  1. Stanford Univ., Stanford, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  3. Arizona State Univ., Tempe, AZ (United States)
  4. Japan Synchrotron Radiation Research Institute (JASRI) (Japan)
  5. RIKEN SPring-8 Center (Japan)
  6. Stanford Univ., Stanford, CA (United States); SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1348987
Grant/Contract Number:
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
IUCrJ
Additional Journal Information:
Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2052-2525
Publisher:
International Union of Crystallography
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; 74 ATOMIC AND MOLECULAR PHYSICS; angular photon correlations; solution diffraction; XFELs; correlated X-ray scattering; gold nanoparticles

Citation Formats

Mendez, Derek, Watkins, Herschel, Qiao, Shenglan, Raines, Kevin S., Lane, Thomas J., Schenk, Gundolf, Nelson, Garrett, Subramanian, Ganesh, Tono, Kensuke, Joti, Yasumasa, Yabashi, Makina, Ratner, Daniel, and Doniach, Sebastian. Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure. United States: N. p., 2016. Web. doi:10.1107/S2052252516013956.
Mendez, Derek, Watkins, Herschel, Qiao, Shenglan, Raines, Kevin S., Lane, Thomas J., Schenk, Gundolf, Nelson, Garrett, Subramanian, Ganesh, Tono, Kensuke, Joti, Yasumasa, Yabashi, Makina, Ratner, Daniel, & Doniach, Sebastian. Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure. United States. doi:10.1107/S2052252516013956.
Mendez, Derek, Watkins, Herschel, Qiao, Shenglan, Raines, Kevin S., Lane, Thomas J., Schenk, Gundolf, Nelson, Garrett, Subramanian, Ganesh, Tono, Kensuke, Joti, Yasumasa, Yabashi, Makina, Ratner, Daniel, and Doniach, Sebastian. 2016. "Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure". United States. doi:10.1107/S2052252516013956. https://www.osti.gov/servlets/purl/1348987.
@article{osti_1348987,
title = {Angular correlations of photons from solution diffraction at a free-electron laser encode molecular structure},
author = {Mendez, Derek and Watkins, Herschel and Qiao, Shenglan and Raines, Kevin S. and Lane, Thomas J. and Schenk, Gundolf and Nelson, Garrett and Subramanian, Ganesh and Tono, Kensuke and Joti, Yasumasa and Yabashi, Makina and Ratner, Daniel and Doniach, Sebastian},
abstractNote = {During X-ray exposure of a molecular solution, photons scattered from the same molecule are correlated. If molecular motion is insignificant during exposure, then differences in momentum transfer between correlated photons are direct measurements of the molecular structure. In conventional small- and wide-angle solution scattering, photon correlations are ignored. This report presents advances in a new biomolecular structural analysis technique, correlated X-ray scattering (CXS), which uses angular intensity correlations to recover hidden structural details from molecules in solution. Due to its intense rapid pulses, an X-ray free electron laser (XFEL) is an excellent tool for CXS experiments. A protocol is outlined for analysis of a CXS data set comprising a total of half a million X-ray exposures of solutions of small gold nanoparticles recorded at the Spring-8 Ångström Compact XFEL facility (SACLA). From the scattered intensities and their correlations, two populations of nanoparticle domains within the solution are distinguished: small twinned, and large probably non-twinned domains. Finally, it is shown analytically how, in a solution measurement, twinning information is only accessible via intensity correlations, demonstrating how CXS reveals atomic-level information from a disordered solution of like molecules.},
doi = {10.1107/S2052252516013956},
journal = {IUCrJ},
number = 6,
volume = 3,
place = {United States},
year = 2016,
month = 9
}

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