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Title: Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion

Abstract

Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with a temporal and spatial resolution of 30 fs and 0.3 Å. This high fidelity is due to interference between the nonstationary excitation and the stationary initial charge distribution. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on ångstrom and femtosecond scales. This x-ray interference has not been employed to image internal motion in molecules before. In conclusion, coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [2]
  1. SLAC National Accelerator Lab., Menlo Park, CA (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States). Photon Ultrafast Laser Science and Engineering Inst. (PULSE)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1331202
Alternate Identifier(s):
OSTI ID: 1328450; OSTI ID: 1348859
Report Number(s):
SLAC-PUB-16830
Journal ID: ISSN 0031-9007; PRLTAO; TRN: US1700170
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Physical Review Letters
Additional Journal Information:
Journal Volume: 117; Journal Issue: 15; Journal ID: ISSN 0031-9007
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
73 NUCLEAR PHYSICS AND RADIATION PHYSICS; 46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY

Citation Formats

Glownia, J. M., Natan, A., Cryan, J. P., Hartsock, R., Kozina, M., Minitti, M. P., Nelson, S., Robinson, J., Sato, T., van Driel, T., Welch, G., Weninger, C., Zhu, D., and Bucksbaum, P. H. Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion. United States: N. p., 2016. Web. doi:10.1103/PhysRevLett.117.153003.
Glownia, J. M., Natan, A., Cryan, J. P., Hartsock, R., Kozina, M., Minitti, M. P., Nelson, S., Robinson, J., Sato, T., van Driel, T., Welch, G., Weninger, C., Zhu, D., & Bucksbaum, P. H. Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion. United States. doi:10.1103/PhysRevLett.117.153003.
Glownia, J. M., Natan, A., Cryan, J. P., Hartsock, R., Kozina, M., Minitti, M. P., Nelson, S., Robinson, J., Sato, T., van Driel, T., Welch, G., Weninger, C., Zhu, D., and Bucksbaum, P. H. Mon . "Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion". United States. doi:10.1103/PhysRevLett.117.153003. https://www.osti.gov/servlets/purl/1331202.
@article{osti_1331202,
title = {Self-referenced coherent diffraction x-ray movie of Ångstrom- and femtosecond-scale atomic motion},
author = {Glownia, J. M. and Natan, A. and Cryan, J. P. and Hartsock, R. and Kozina, M. and Minitti, M. P. and Nelson, S. and Robinson, J. and Sato, T. and van Driel, T. and Welch, G. and Weninger, C. and Zhu, D. and Bucksbaum, P. H.},
abstractNote = {Time-resolved femtosecond x-ray diffraction patterns from laser-excited molecular iodine are used to create a movie of intramolecular motion with a temporal and spatial resolution of 30 fs and 0.3 Å. This high fidelity is due to interference between the nonstationary excitation and the stationary initial charge distribution. The initial state is used as the local oscillator for heterodyne amplification of the excited charge distribution to retrieve real-space movies of atomic motion on ångstrom and femtosecond scales. This x-ray interference has not been employed to image internal motion in molecules before. In conclusion, coherent vibrational motion and dispersion, dissociation, and rotational dephasing are all clearly visible in the data, thereby demonstrating the stunning sensitivity of heterodyne methods.},
doi = {10.1103/PhysRevLett.117.153003},
journal = {Physical Review Letters},
number = 15,
volume = 117,
place = {United States},
year = {Mon Oct 03 00:00:00 EDT 2016},
month = {Mon Oct 03 00:00:00 EDT 2016}
}

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Cited by: 29 works
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Works referenced in this record:

Optical control of molecular dynamics: Molecular cannons, reflectrons, and wave‐packet focusers
journal, November 1993

  • Krause, Jeffrey L.; Whitnell, Robert M.; Wilson, Kent R.
  • The Journal of Chemical Physics, Vol. 99, Issue 9, p. 6562-6578
  • DOI: 10.1063/1.465848