Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Coulomb explosion imaging of CH3I and CH2ClI photodissociation dynamics

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.5041381· OSTI ID:1610037
 [1];  [2];  [2];  [3];  [2];  [4];  [3];  [3];  [5];  [6];  [3];  [3];  [7];  [7];  [2];  [5];  [6];  [8];  [6];  [9] more »;  [6];  [10];  [9];  [2];  [9];  [2];  [3];  [4];  [2];  [6];  [11];  [6];  [12];  [5];  [7];  [13];  [3];  [6];  [3];  [14];  [15];  [6];  [10];  [16];  [2];  [10];  [13];  [2];  [6];  [13] « less
  1. Univ. of Oxford (United Kingdom); DOE/OSTI
  2. Univ. of Oxford (United Kingdom)
  3. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  4. Saint-Petersburg State Univ. (Russia)
  5. Max-Born-Inst., Berlin (Germany)
  6. Sorbonne Univ., Paris (France)
  7. Univ. Paris-Saclay, Gif-sur-Yvette (France)
  8. Science and Technology Facilities Council (STFC), Daresbury (United Kingdom). Daresbury Lab.
  9. Lund Univ. (Sweden)
  10. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Univ. of Hamburg (Germany)
  11. Sorbonne Univ., Paris (France); Uppsala Univ. (Sweden)
  12. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); European X-ray Free-Electron Laser (XFEL), Hamburg (Germany)
  13. Kansas State Univ., Manhattan, KS (United States)
  14. Aarhus Univ. (Denmark)
  15. Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany); Max Planck Inst. for Biophysical Chemistry, Göttingen (Germany); Göttingen Univ. (Germany)
  16. Univ. College London, Bloomsbury (United Kingdom)

The photodissociation dynamics of CH3I and CH2ClI at 272 nm were investigated by time-resolved Coulomb explosion imaging, with an intense non-resonant 815 nm probe pulse. Fragment ion momenta over a wide m/z range were recorded simultaneously by coupling a velocity map imaging spectrometer with a pixel imaging mass spectrometry camera. For both molecules, delay-dependent pump-probe features were assigned to ultraviolet-induced carbon-iodine bond cleavage followed by Coulomb explosion. Multi-mass imaging also allowed the sequential cleavage of both carbon-halogen bonds in CH2ClI to be investigated. Furthermore, delay-dependent relative fragment momenta of a pair of ions were directly determined using recoil-frame covariance analysis. These results are complementary to conventional velocity map imaging experiments and demonstrate the application of time-resolved Coulomb explosion imaging to photoinduced real-time molecular motion.

Research Organization:
Kansas State Univ., Manhattan, KS (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division; German Research Council (DFG); Swedish Research Council; Swedish Foundation for Strategic Research
Grant/Contract Number:
FG02-86ER13491
OSTI ID:
1610037
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 20 Vol. 149; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

References (71)

Picosecond excitation and TRANS-CIS isomerization of stilbene in a supersonic jet: Dynamics and spectra journal May 1982
Photodissociation channels and energy partitioning in the photofragmentation of alkyl iodides journal May 1988
Competitive photodecomposition reactions of chloroiodomethane journal February 1987
Cl∗(2P1/2) production dynamics from chloroiodomethane (CH2ICl) in the ultraviolet journal August 2004
A 40-fs time-resolved absorption study on cis-stilbene in solution: observation of wavepacket motion on the reactive excited state journal November 2004
Femtosecond photodissociation dynamics of chloroiodomethane in the first absorption band journal September 2017
Large-format, high-speed, X-ray pnCCDs combined with electron and ion imaging spectrometers in a multipurpose chamber for experiments at 4th generation light sources
  • Strüder, Lothar; Epp, Sascha; Rolles, Daniel
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 614, Issue 3 https://doi.org/10.1016/j.nima.2009.12.053
journal March 2010
Pixel imaging mass spectrometry with fast silicon detectors
  • Nomerotski, A.; Adigun-Boaye, S.; Brouard, M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 633 https://doi.org/10.1016/j.nima.2010.06.178
journal May 2011
The FLASH pump–probe laser system: Setup, characterization and optical beamlines
  • Redlin, H.; Al-Shemmary, A.; Azima, A.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 635, Issue 1 https://doi.org/10.1016/j.nima.2010.09.159
journal April 2011
Photofragment imaging: The 266 nm photodissociation of CH3I journal March 1989
Photodissociation of a molecule with two chromophores. Bromoiodomethane journal March 1982
Emission spectroscopy of photodissociating methyl iodide and methyl-d3 iodide journal October 1986
Femtochemistry:  Atomic-Scale Dynamics of the Chemical Bond journal June 2000
Photodissociation Dynamics of CH 2 ICl at 222, 236, 266, 280, and ∼304 nm journal September 2002
Velocity Map Imaging and Theoretical Study of the Coulomb Explosion of CH 3 I under Intense Femtosecond IR Pulses journal November 2011
Velocity Map Imaging of Dissociative Ionization and Coulomb Explosion of CH 3 I Induced by a Femtosecond Laser journal May 2008
Femtosecond Time-Resolved UV−Visible Absorption Spectroscopy of trans -Azobenzene in Solution journal January 1996
Femtosecond Real-Time Probing of Reactions. 23. Studies of Temporal, Velocity, Angular, and State Dynamics from Transition States to Final Products by Femtosecond-Resolved Mass Spectrometry journal June 1998
Photoelectron and Photofragment Velocity Imaging Following the Excitation of CH 3 I to the A-Band Using fs, ps, and ns Laser Pulses journal August 1999
Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging journal December 2016
nσ* and πσ* excited states in aryl halide photochemistry: a comprehensive study of the UV photodissociation dynamics of iodobenzene journal January 2011
Dynamics of the A-band ultraviolet photodissociation of methyl iodide and ethyl iodide via velocity-map imaging with ‘universal’ detection journal January 2015
Photodissociation dynamics of ICH 2 Cl → CH 2 Cl + I*/I: photofragment translational spectroscopy at 304 and 277 nm journal January 2016
Halogen-atom effect on the ultrafast photodissociation dynamics of the dihalomethanes CH 2 ICl and CH 2 BrI journal January 2018
Excited fragments from excited molecules: energy partitioning in the photodissociation of alkyl iodides journal January 1972
Velocity map imaging of ions and electrons using electrostatic lenses: Application in photoelectron and photofragment ion imaging of molecular oxygen journal September 1997
Photodissociation of C6H5I, C6F5I, and related iodides in the ultraviolet journal August 2002
Two-dimensional charged particle image inversion using a polar basis function expansion journal November 2004
A 193nm laser photofragmentation time-of-flight mass spectrometric study of chloroiodomethane journal November 2005
Femtosecond multichannel photodissociation dynamics of CH3I from the A band by velocity map imaging journal January 2007
The photodissociation of CH3I in the red edge of the A-band: Comparison between slice imaging experiments and multisurface wave packet calculations journal November 2009
The electronic state‐selective photodissociation of CH2BrI at 248, 210, and 193 nm journal February 1987
A b i n i t i o potential energy surfaces and trajectory studies of A ‐band photodissociation dynamics: CH 3 I*→CH 3 +I and CH 3 +I* journal April 1991
Control and femtosecond time-resolved imaging of torsion in a chiral molecule journal May 2012
Methyl iodide A-band decomposition study by photofragment velocity imaging journal September 1998
Energy partitioning following photodissociation of methyl iodide in the A band: A velocity mapping study journal January 1999
Charge transfer in dissociating iodomethane and fluoromethane molecules ionized by intense femtosecond X-ray pulses journal March 2016
Communication: Three-fold covariance imaging of laser-induced Coulomb explosions journal April 2016
Photodissociation of aligned CH 3 I and C 6 H 3 F 2 I molecules probed with time-resolved Coulomb explosion imaging by site-selective extreme ultraviolet ionization journal January 2018
Communication: Gas-phase structural isomer identification by Coulomb explosion of aligned molecules journal March 2018
The dynamics of small molecules in intense laser fields journal April 2004
Ultrafast mapping of H 2 + (D 2 + ) nuclear wave packets using time-resolved Coulomb explosion imaging journal June 2006
Laser Coulomb explosion imaging for probing ultra-fast molecular dynamics journal June 2006
Towards imaging of ultrafast molecular dynamics using FELs journal August 2013
Femtosecond x-ray photoelectron diffraction on gas-phase dibromobenzene molecules journal June 2014
Covariance mapping techniques journal July 2016
PImMS, a fast event-triggered monolithic pixel detector with storage of multiple timestamps journal August 2012
Microwave Determination of the Molecular Structures and Nuclear Couplings of the Methyl Halides journal August 1948
Time-resolved Coulomb explosion imaging: A method to measure structure and dynamics of molecular nuclear wave packets journal July 1998
Time-resolved Coulomb-explosion imaging of nuclear wave-packet dynamics induced in diatomic molecules by intense few-cycle laser pulses journal January 2011
Covariance imaging experiments using a pixel-imaging mass-spectrometry camera journal January 2014
Coulomb-explosion imaging using a pixel-imaging mass-spectrometry camera journal May 2015
Coulomb-explosion imaging of concurrent CH 2 BrI photodissociation dynamics journal October 2017
Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom journal April 2018
Transient X-Ray Fragmentation: Probing a Prototypical Photoinduced Ring Opening journal June 2012
Dynamic Stark Control of Torsional Motion by a Pair of Laser Pulses journal August 2014
Imaging Molecular Motion: Femtosecond X-Ray Scattering of an Electrocyclic Chemical Reaction journal June 2015
Wave Packet Structure and Dynamics Measured by Coulomb Explosion journal May 1995
Time-Resolved Imaging and Manipulation of H 2 Fragmentation in Intense Laser Fields journal August 2005
CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser journal August 2018
Direct Determination of Absolute Molecular Stereochemistry in Gas Phase by Coulomb Explosion Imaging journal September 2013
Imaging charge transfer in iodomethane upon x-ray photoabsorption journal July 2014
Coulomb Explosion Imaging of Small Molecules journal April 1989
Covariance Mapping: A Correlation Method Applied to Multiphoton Multiple Ionization journal November 1989
Dissociative ionization and Coulomb explosion of CH3I in intense femto second laser fields journal June 2017
Identification of absolute geometries of cis and trans molecular isomers by Coulomb Explosion Imaging text January 2016
Coulomb-explosion imaging of concurrent CH$_{2}$BrI photodissociation dynamics text January 2017
Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom 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
Direct observation of charge separation in an organic light harvesting system by femtosecond time-resolved XPS text January 2021
CAMP@FLASH: an end-station for imaging, electron- and ion-spectroscopy, and pump–probe experiments at the FLASH free-electron laser text January 2018

Cited By (4)

Time-resolved imaging of bound and dissociating nuclear wave packets in strong-field ionized iodomethane journal January 2019
Multi-mass velocity-map imaging studies of photoinduced and electron-induced chemistry journal January 2019
Photodissociation dynamics of CH 3 I probed via multiphoton ionisation photoelectron spectroscopy journal January 2019
Threshold photodissociation dynamics of NO 2 studied by time-resolved cold target recoil ion momentum spectroscopy journal November 2019

Similar Records

Coulomb-explosion imaging of concurrent CH2BrI photodissociation dynamics
Journal Article · Tue Oct 17 00:00:00 EDT 2017 · Physical Review A · OSTI ID:1540659

Single- and multi-photon-induced ultraviolet excitation and photodissociation of CH3I probed by coincident ion momentum imaging
Journal Article · Thu Mar 16 00:00:00 EDT 2023 · Physical Chemistry Chemical Physics. PCCP · OSTI ID:2006863