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.
- 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}
}
Free Publicly Available Full Text
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DOI: 10.1073/pnas.1816730116
DOI: 10.1073/pnas.1816730116
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