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Title: Diffractive Imaging of C60 Structural Deformations Induced by Intense Femtosecond Midinfrared Laser Fields

Journal Article · · Physical Review Letters
 [1];  [2];  [2];  [3];  [2];  [4];  [5];  [6];  [2];  [3];  [3];  [3];  [7];  [2]
  1. Ludwig Maximilian Univ. of Munich, Munich (Germany); Max Planck Institute of Quantum Optics, Garching (Germany); DOE/OSTI
  2. The Ohio State Univ., Columbus, OH (United States)
  3. Tohoku Univ., Sendai (Japan)
  4. Ludwig Maximilian Univ. of Munich, Munich (Germany); Max Planck Institute of Quantum Optics, Garching (Germany)
  5. Ludwig Maximilian Univ. of Munich, Munich (Germany); Kansas State Univ., Manhattan, KS (United States); East China Normal University, Shanghai (China)
  6. Ludwig Maximilian Univ. of Munich, Munich (Germany); Max Planck Institute of Quantum Optics, Garching (Germany); Univ. of Warsaw (Poland)
  7. Ludwig Maximilian Univ. of Munich, Munich (Germany); Max Planck Institute of Quantum Optics, Garching (Germany); Kansas State Univ., Manhattan, KS (United States)
+ Show Author Affiliations

Theoretical studies indicated that C60 exposed to linearly polarized intense infrared pulses undergoes periodic cage structural distortions with typical periods around 100 fs (1 fs = 10–15 s). Here, we use the laser-driven self-imaging electron diffraction technique, previously developed for atoms and small molecules, to measure laser-induced deformation of C60 in an intense 3.6 μm laser field. A prolate molecular elongation along the laser polarization axis is determined to be (6.1 ± 1.4)% via both angular- and energy-resolved measurements of electrons that are released, driven back, and diffracted from the molecule within the same laser field. The observed deformation is confirmed by density functional theory simulations of nuclear dynamics on time-dependent adiabatic states and indicates a nonadiabatic excitation of the hg(1) prolate-oblate mode. Here, the results demonstrate the applicability of laser-driven electron diffraction methods for studying macromolecular structural dynamics in four dimensions with atomic time and spatial resolutions.

Research Organization:
Kansas State Univ., Manhattan, KS (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES); German Research Foundation (DFG); European Research Council (ERC); Japan Society for the Promotion of Science (JSPS); US Air Force Office of Scientific Research (AFOSR); Ministry of Education, Culture, Sports, Science and Technology (MEXT)
Grant/Contract Number:
FG02-86ER13491; FG02-04ER15614
OSTI ID:
1610050
Journal Information:
Physical Review Letters, Journal Name: Physical Review Letters Journal Issue: 5 Vol. 122; ISSN 0031-9007
Publisher:
American Physical Society (APS)Copyright Statement
Country of Publication:
United States
Language:
English

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Setting the photoelectron clock through molecular alignment text January 2020

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