skip to main content

DOE PAGESDOE PAGES

This content will become publicly available on July 8, 2019

Title: Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction

The ultrafast spontaneous electron-density fluctuation dynamics in molecules is studied theoretically by off-resonant multiple X-ray diffraction events. The time- and wavevector-resolved photon-coincidence signals give an image of electron-density fluctuations expressed through the four-point correlation function of the charge density in momentum space. A Fourier transform of the signal provides a real-space image of the multipoint charge-density correlation functions, which reveal snapshots of the evolving electron density in between the diffraction events. The proposed technique is illustrated by ab initio simulations of the momentum- and real-space inelastic scattering signals from a linear cyanotetracetylene molecule.
Authors:
; ; ; ORCiD logo
Publication Date:
Grant/Contract Number:
FG02-04ER15571
Type:
Published Article
Journal Name:
Proceedings of the National Academy of Sciences of the United States of America
Additional Journal Information:
Journal Name: Proceedings of the National Academy of Sciences of the United States of America Journal Volume: 116 Journal Issue: 2; Journal ID: ISSN 0027-8424
Publisher:
Proceedings of the National Academy of Sciences
Sponsoring Org:
USDOE
Country of Publication:
United States
Language:
English
OSTI Identifier:
1488766

Ye, Lyuzhou, Rouxel, Jérémy R., Cho, Daeheum, and Mukamel, Shaul. Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction. United States: N. p., Web. doi:10.1073/pnas.1816730116.
Ye, Lyuzhou, Rouxel, Jérémy R., Cho, Daeheum, & Mukamel, Shaul. Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction. United States. doi:10.1073/pnas.1816730116.
Ye, Lyuzhou, Rouxel, Jérémy R., Cho, Daeheum, and Mukamel, Shaul. 2018. "Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction". United States. doi:10.1073/pnas.1816730116.
@article{osti_1488766,
title = {Imaging electron-density fluctuations by multidimensional X-ray photon-coincidence diffraction},
author = {Ye, Lyuzhou and Rouxel, Jérémy R. and Cho, Daeheum and Mukamel, Shaul},
abstractNote = {The ultrafast spontaneous electron-density fluctuation dynamics in molecules is studied theoretically by off-resonant multiple X-ray diffraction events. The time- and wavevector-resolved photon-coincidence signals give an image of electron-density fluctuations expressed through the four-point correlation function of the charge density in momentum space. A Fourier transform of the signal provides a real-space image of the multipoint charge-density correlation functions, which reveal snapshots of the evolving electron density in between the diffraction events. The proposed technique is illustrated by ab initio simulations of the momentum- and real-space inelastic scattering signals from a linear cyanotetracetylene molecule.},
doi = {10.1073/pnas.1816730116},
journal = {Proceedings of the National Academy of Sciences of the United States of America},
number = 2,
volume = 116,
place = {United States},
year = {2018},
month = {12}
}

Works referenced in this record:

Density?functional thermochemistry. III. The role of exact exchange
journal, April 1993
  • Becke, Axel D.
  • The Journal of Chemical Physics, Vol. 98, Issue 7, p. 5648-5652
  • DOI: 10.1063/1.464913

NWChem: A comprehensive and scalable open-source solution for large scale molecular simulations
journal, September 2010
  • Valiev, M.; Bylaska, E. J.; Govind, N.
  • Computer Physics Communications, Vol. 181, Issue 9, p. 1477-1489
  • DOI: 10.1016/j.cpc.2010.04.018

A new hybrid exchange�correlation functional using the Coulomb-attenuating method (CAM-B3LYP)
journal, July 2004
  • Yanai, Takeshi; Tew, David P.; Handy, Nicholas C.
  • Chemical Physics Letters, Vol. 393, Issue 1-3, p. 51-57
  • DOI: 10.1016/j.cplett.2004.06.011

Ab Initio Calculation of Vibrational Absorption and Circular Dichroism Spectra Using Density Functional Force Fields
journal, November 1994
  • Stephens, P. J.; Devlin, F. J.; Chabalowski, C. F.
  • The Journal of Physical Chemistry, Vol. 98, Issue 45, p. 11623-11627
  • DOI: 10.1021/j100096a001