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Title: Diffractive imaging of a rotational wavepacket in nitrogen molecules with femtosecond megaelectronvolt electron pulses

Imaging changes in molecular geometries on their natural femtosecond timescale with sub-Angström spatial precision is one of the critical challenges in the chemical sciences, as the nuclear geometry changes determine the molecular reactivity. For photoexcited molecules, the nuclear dynamics determine the photoenergy conversion path and efficiency. Here we report a gas-phase electron diffraction experiment using megaelectronvolt (MeV) electrons, where we captured the rotational wavepacket dynamics of nonadiabatically laser-aligned nitrogen molecules. We achieved a combination of 100 fs root-mean-squared temporal resolution and sub-Angstrom (0.76 Å) spatial resolution that makes it possible to resolve the position of the nuclei within the molecule. In addition, the diffraction patterns reveal the angular distribution of the molecules, which changes from prolate (aligned) to oblate (anti-aligned) in 300 fs. Lastly, our results demonstrate a significant and promising step towards making atomically resolved movies of molecular reactions.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] ;  [3] more »;  [3] ;  [1] ;  [3] « less
  1. Univ. of Nebraska-Lincoln, Lincoln, NE (United States)
  2. SLAC National Accelerator Lab., Menlo Park, CA (United States); Potsdam Univ., Potsdam (Germany)
  3. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
OSTI Identifier:
1251412
Grant/Contract Number:
AC02-76SF00515
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND TECHNOLOGY chemical sciences; optical sciences