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

Abstract

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. Finally, 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:
Research Org.:
Univ. of California, Irvine, CA (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; National Science Foundation (NSF)
OSTI Identifier:
1488766
Alternate Identifier(s):
OSTI ID: 1609514
Grant/Contract Number:  
FG02-04ER15571; SC0019484; CHE-1663822
Resource 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:
National Academy of Sciences
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS; x-ray diffraction; photon-coincidence; multidimensional spectroscopy

Citation Formats

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., 2018. 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. Mon . "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. Finally, 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}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
DOI: 10.1073/pnas.1816730116

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Cited by: 1 work
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Works referenced in this record:

Single-shot three-dimensional structure determination of nanocrystals with femtosecond X-ray free-electron laser pulses
journal, June 2014

  • Xu, Rui; Jiang, Huaidong; Song, Changyong
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5061

X-ray imaging beyond the limits
journal, April 2009


Laboratory detection of HC9N using a Fourier transform microwave spectrometer
journal, April 1991

  • Iida, Minoru; Ohshima, Yasuhiro; Endo, Yasuki
  • The Astrophysical Journal, Vol. 371
  • DOI: 10.1086/185998

X-rays inspire electron movies
journal, October 2012


Monitoring molecular nonadiabatic dynamics with femtosecond X-ray diffraction
journal, June 2018

  • Bennett, Kochise; Kowalewski, Markus; Rouxel, Jérémy R.
  • Proceedings of the National Academy of Sciences, Vol. 115, Issue 26
  • DOI: 10.1073/pnas.1805335115

Extending the methodology of X-ray crystallography to allow imaging of micrometre-sized non-crystalline specimens
journal, July 1999

  • Miao, Jianwei; Charalambous, Pambos; Kirz, Janos
  • Nature, Vol. 400, Issue 6742
  • DOI: 10.1038/22498

Femtosecond X-ray coherent diffraction of aligned amyloid fibrils on low background graphene
journal, May 2018

  • Seuring, Carolin; Ayyer, Kartik; Filippaki, Eleftheria
  • Nature Communications, Vol. 9, Article No. 1836
  • DOI: 10.1038/s41467-018-04116-9

Time-Resolved X-Ray Imaging of Anisotropic Nanoplasma Expansion
journal, September 2014


Cryogenic Photochemical Synthesis and Electronic Spectroscopy of Cyanotetracetylene
journal, September 2017

  • Szczepaniak, Urszula; Kołos, Robert; Gronowski, Marcin
  • The Journal of Physical Chemistry A, Vol. 121, Issue 39
  • DOI: 10.1021/acs.jpca.7b07849

Beyond crystallography: Diffractive imaging using coherent x-ray light sources
journal, April 2015


Non-linear non-local molecular electrodynamics with nano-optical fields
journal, October 2015

  • Chernyak, Vladimir Y.; Saurabh, Prasoon; Mukamel, Shaul
  • The Journal of Chemical Physics, Vol. 143, Issue 16
  • DOI: 10.1063/1.4934231

Linear-Response and Real-Time Time-Dependent Density Functional Theory Studies of Core-Level Near-Edge X-Ray Absorption
journal, August 2012

  • Lopata, K.; Van Kuiken, B. E.; Khalil, M.
  • Journal of Chemical Theory and Computation, Vol. 8, Issue 9
  • DOI: 10.1021/ct3005613

Ultrafast Time-Resolved Transient Structures of Solids and Liquids Studied by Means of X-ray Diffraction and EXAFS
journal, August 1999

  • Tomov, Ivan V.; Oulianov, Dmitri A.; Chen, Peilin
  • The Journal of Physical Chemistry B, Vol. 103, Issue 34
  • DOI: 10.1021/jp9908449

Correlation and the density-matrix approach to inelastic electron holography in solid state plasmas
journal, January 2005


Phase retrieval of diffraction patterns from noncrystalline samples using the oversampling method
journal, May 2003


Post-sample aperture for low background diffraction experiments at X-ray free-electron lasers
journal, October 2017

  • Wiedorn, Max O.; Awel, Salah; Morgan, Andrew J.
  • Journal of Synchrotron Radiation, Vol. 24, Issue 6
  • DOI: 10.1107/S1600577517011961

Phase retrieval by iterated projections
journal, January 2003


Attosecond time–energy structure of X-ray free-electron laser pulses
journal, March 2018


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

Nonlinear light scattering in molecules triggered by an impulsive x-ray Raman process
journal, May 2013


Current Status of Single Particle Imaging with X-ray Lasers
journal, January 2018

  • Sun, Zhibin; Fan, Jiadong; Li, Haoyuan
  • Applied Sciences, Vol. 8, Issue 1
  • DOI: 10.3390/app8010132

Femtosecond X-ray-induced explosion of C60 at extreme intensity
journal, June 2014

  • Murphy, B. F.; Osipov, T.; Jurek, Z.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5281

Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction
journal, June 2015


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

Revealing Three-Dimensional Structure of an Individual Colloidal Crystal Grain by Coherent X-Ray Diffractive Imaging
journal, September 2016


A theoretical systematic study of a series of isocyanopolyynes
journal, October 2013

  • Vichietti, R. M.; Haiduke, R. L. A.
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 114
  • DOI: 10.1016/j.saa.2013.05.066

Probing electronic and vibrational dynamics in molecules by time-resolved photoelectron, Auger-electron, and X-ray photon scattering spectroscopy
journal, January 2015

  • Bennett, Kochise; Kowalewski, Markus; Mukamel, Shaul
  • Faraday Discussions, Vol. 177
  • DOI: 10.1039/C4FD00178H

SACLA hard-X-ray compact FEL
journal, July 2012


Broken translational and rotational symmetry via charge stripe order in underdoped YBa2Cu3O6+y
journal, March 2015


Time-, frequency-, and wavevector-resolved x-ray diffraction from single molecules
journal, May 2014

  • Bennett, Kochise; Biggs, Jason D.; Zhang, Yu
  • The Journal of Chemical Physics, Vol. 140, Issue 20
  • DOI: 10.1063/1.4878377

Generation of High-Power High-Intensity Short X-Ray Free-Electron-Laser Pulses
journal, January 2018


Low Temperature Synthesis and Phosphorescence of Methylcyanotriacetylene
journal, December 2017

  • Szczepaniak, Urszula; Kołos, Robert; Gronowski, Marcin
  • The Journal of Physical Chemistry A, Vol. 122, Issue 1
  • DOI: 10.1021/acs.jpca.7b09728

Coherent-Pulse 2D Crystallography Using a Free-Electron Laser X-Ray Source
journal, January 2009


X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser
journal, February 2014


The infrared fundamental intensities of some cyanopolyynes
journal, May 2012

  • Vichietti, Rafael M.; Haiduke, Roberto L. A.
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 90
  • DOI: 10.1016/j.saa.2012.01.005

X-Ray Sum Frequency Diffraction for Direct Imaging of Ultrafast Electron Dynamics
journal, June 2018


Impact of hollow-atom formation on coherent x-ray scattering at high intensity
journal, March 2011


Femtosecond x-ray crystallography
journal, January 2001

  • Rousse, Antoine; Rischel, Christian; Gauthier, Jean-Claude
  • Reviews of Modern Physics, Vol. 73, Issue 1
  • DOI: 10.1103/RevModPhys.73.17

Experimental Structures of the Carbon Chains HC7N, HC9N, and HC11N by Isotopic Substitution
journal, September 2000

  • McCarthy, M. C.; Levine, E. S.; Apponi, A. J.
  • Journal of Molecular Spectroscopy, Vol. 203, Issue 1
  • DOI: 10.1006/jmsp.2000.8149

Isotope scrambling in the formation of cyanopolyynes by laser ablation of carbon particles in liquid acetonitrile
journal, January 2012


Time-dependent density functional theory within the Tamm–Dancoff approximation
journal, December 1999


Sequential multiphoton multiple ionization of atomic argon and xenon irradiated by x-ray free-electron laser pulses from SACLA
journal, August 2013

  • Motomura, K.; Fukuzawa, H.; Son, S-K
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 46, Issue 16
  • DOI: 10.1088/0953-4075/46/16/164024

Single-molecule X-ray diffraction
journal, October 2000


Parity alternation of interstellar molecules cyanopolyynes HCnN (n=1–17)
journal, October 2009


The detection of HC9N in interstellar space
journal, July 1978

  • Broten, N. W.; Oka, T.; Avery, L. W.
  • The Astrophysical Journal, Vol. 223
  • DOI: 10.1086/182739

Multidimensional scattering of attosecond x-ray pulses detected by photon-coincidence
journal, June 2014

  • Biggs, Jason D.; Bennett, Kochise; Zhang, Yu
  • Journal of Physics B: Atomic, Molecular and Optical Physics, Vol. 47, Issue 12
  • DOI: 10.1088/0953-4075/47/12/124037

Towards hybrid pixel detectors for energy-dispersive or soft X-ray photon science
journal, February 2016

  • Jungmann-Smith, J. H.; Bergamaschi, A.; Brückner, M.
  • Journal of Synchrotron Radiation, Vol. 23, Issue 2
  • DOI: 10.1107/S1600577515023541

Picosecond–milliångström lattice dynamics measured by ultrafast X-ray diffraction
journal, March 1999

  • Rose-Petruck, Christoph; Jimenez, Ralph; Guo, Ting
  • Nature, Vol. 398, Issue 6725
  • DOI: 10.1038/18631

Self-Referenced Coherent Diffraction X-Ray Movie of Ångstrom- and Femtosecond-Scale Atomic Motion
journal, October 2016


Carbon chains and rings in the laboratory and in space
journal, March 2001

  • Thaddeus, P.; McCarthy, M. C.
  • Spectrochimica Acta Part A: Molecular and Biomolecular Spectroscopy, Vol. 57, Issue 4
  • DOI: 10.1016/S1386-1425(00)00442-X

Time-resolved x-ray spectroscopies: Nonlinear response functions and Liouville-space pathways
journal, May 2001


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

X-ray Scattering Studies of Protein Structural Dynamics
journal, May 2017


Hanbury Brown–Twiss Interferometry at a Free-Electron Laser
journal, July 2013