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

Journal Article · · Physical Review Letters
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  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)

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.

Research Organization:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Stanford PULSE Institute, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-76SF00515
OSTI ID:
1331202
Alternate ID(s):
OSTI ID: 1328198
OSTI ID: 1328450
OSTI ID: 1348859
Report Number(s):
SLAC-PUB--16830
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 15 Vol. 117; ISSN 0031-9007; ISSN PRLTAO
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

References (39)

Femtosecond Time-Resolved Photoelectron Spectroscopy journal June 2004
Direct imaging of excited electronic states using diffraction techniques: theoretical considerations journal November 1996
CSPAD-140k: A versatile detector for LCLS experiments
  • Herrmann, Sven; Boutet, Sébastien; Duda, Brian
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 718 https://doi.org/10.1016/j.nima.2013.01.057
journal August 2013
Femtosecond Time-Resolved Photoelectron Spectroscopy journal April 2004
On the Theory of Time-Resolved X-ray Diffraction journal January 2008
Ultrafast X-ray and Electron Diffraction:  Theoretical Considerations journal November 1997
Ultrafast X-ray Diffraction Theory journal November 1998
Imaging ultrafast molecular dynamics with laser-induced electron diffraction journal March 2012
Serial time-resolved crystallography of photosystem II using a femtosecond X-ray laser journal July 2014
Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses journal April 2016
Ultrafast X-ray Auger probing of photoexcited molecular dynamics journal June 2014
X-rays inspire electron movies journal October 2012
Fourier-transform inelastic X-ray scattering from time- and momentum-dependent phonon–phonon correlations journal October 2013
Revival structures in picosecond laser-induced alignment of I2 molecules. II. Numerical modeling journal April 2002
Time-resolved x-ray diffraction: Statistical theory and its application to the photo-physics of molecular iodine journal June 2002
Iodine Revisited journal July 1971
Continuous absorption below the band convergence limit in the I2 B ← X transition journal July 1973
Concerted electron and proton transfer in ionic crystals mapped by femtosecond x-ray powder diffraction journal August 2010
Ab initio studies of ultrafast x-ray scattering of the photodissociation of iodine journal September 2010
X-ray spatial frequency heterodyne imaging journal February 2012
Optical control of molecular dynamics: Molecular cannons, reflectrons, and wave‐packet focusers journal November 1993
Imaging electronic quantum motion with light journal July 2012
Observation of femtosecond molecular dynamics via pump–probe gas phase x-ray scattering journal January 2016
Strong-field impulsive alignment in the presence of high temperatures and large centrifugal distortion journal September 2008
Theory of time-resolved inelastic x-ray diffraction journal February 2010
Angle-resolved and internuclear-separation-resolved measurements of the ionization rate of the B state of I 2 by strong laser fields journal October 2011
Femtosecond photoelectron diffraction on laser-aligned molecules: Towards time-resolved imaging of molecular structure journal December 2013
X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser journal February 2014
Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction journal June 2015
Diffractive Imaging of Coherent Nuclear Motion in Isolated Molecules journal October 2016
Experimental Observation of Revival Structures in Picosecond Laser-Induced Alignment of I2 journal September 2001
The X-ray Pump–Probe instrument at the Linac Coherent Light Source journal April 2015
Iodine revisited journal June 2007
Iodine revisited journal June 2007
Femtosecond Time-Resolved Photoelectron Imaging journal May 2006
Experimental Observation of Revival Structures in Picosecond Laser-Induced Alignment of I2 text January 2001
X-Ray Diffraction from Isolated and Strongly Aligned Gas-Phase Molecules with a Free-Electron Laser text January 2014
Absolute absorption cross-section and photolysis rate of I2 journal January 2004
Absolute absorption cross-section and photolysis rate of I2 posted_content May 2004

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