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Title: Photodissociation of aligned CH3I and C6H3F2I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization

Journal Article · · Structural Dynamics
DOI:https://doi.org/10.1063/1.4998648· OSTI ID:1499000
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  1. Univ. of Oxford, Oxford (United Kingdom)
  2. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. Max Born Institute for Nonlinear Optics and Short Pulse Spectroscopy, Berlin (Germany)
  4. Univ. of Connecticut, Storrs, CT (United States)
  5. Aarhus Univ., Aarhus C (Denmark)
  6. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Helmholtz Zentrum Dresden Rossendorf, Dresden (Germany)
  7. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. Hamburg, Hamburg (Germany)
  8. Technische Univ. Berlin, Berlin (Germany)
  9. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Max Planck Institute for Biophysical Chemistry, Gottingen (Germany); Gottingen Univ., Gottingen (Germany)
  10. Lund Univ., Lund (Sweden)
  11. Kansas State Univ., Manhattan, KS (United States)
  12. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Kansas State Univ., Manhattan, KS (United States)
+ Show Author Affiliations

We explore time-resolved Coulomb explosion induced by intense, extreme ultraviolet (XUV) femtosecond pulses from a free-electron laser as a method to image photo-induced molecular dynamics in two molecules, iodomethane and 2,6-difluoroiodobenzene. At an excitation wavelength of 267 nm, the dominant reaction pathway in both molecules is neutral dissociation via cleavage of the carbon–iodine bond. This allows investigating the influence of the molecular environment on the absorption of an intense, femtosecond XUV pulse and the subsequent Coulomb explosion process. We find that the XUV probe pulse induces local inner-shell ionization of atomic iodine in dissociating iodomethane, in contrast to non-selective ionization of all photofragments in difluoroiodobenzene. Here, the results reveal evidence of electron transfer from methyl and phenyl moieties to a multiply charged iodine ion. In addition, indications for ultrafast charge rearrangement on the phenyl radical are found, suggesting that time-resolved Coulomb explosion imaging is sensitive to the localization of charge in extended molecules.

Research Organization:
Kansas State Univ., Manhattan, KS (United States); Univ. of Connecticut, Storrs, CT (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
FG02-86ER13491; SC0012376
OSTI ID:
1499000
Alternate ID(s):
OSTI ID: 1418084
Journal Information:
Structural Dynamics, Vol. 5, Issue 1; ISSN 2329-7778
Publisher:
American Crystallographic Association/AIPCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 34 works
Citation information provided by
Web of Science

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Cited By (8)

Spatiotemporal imaging of valence electron motion journal March 2019
Multi-mass velocity-map imaging studies of photoinduced and electron-induced chemistry journal January 2019
Communication: Gas-phase structural isomer identification by Coulomb explosion of aligned molecules journal March 2018
Coulomb explosion imaging of CH 3 I and CH 2 ClI photodissociation dynamics journal November 2018
CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser text January 2018
CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser text January 2018
Coulomb explosion imaging of $CH_{3}I$ and $C_{2}ClI$ photodissociation dynamics text January 2018
Spatiotemporal imaging of valence electron motion text January 2019

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Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
Free electron lasers
Photodissociation
Photoionization
X-rays
Reaction mechanisms
Ultraviolet optics
Chemical compounds and components
Chemical elements
Molecular dynamics
Surface collisions