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

Time-resolved Auger–Meitner spectroscopy of the photodissociation dynamics of CS2

Journal Article · · Journal of Physics. B, Atomic, Molecular and Optical Physics
 [1];  [2];  [3];  [2];  [4];  [2];  [5];  [6];  [2];  [7];  [2];  [8];  [8];  [9];  [4];  [7];  [10];  [11];  [2];  [12] more »;  [13];  [2];  [9];  [14];  [8];  [15];  [2];  [1];  [15] « less
  1. University of Southampton (United Kingdom)
  2. Elettra—Sincrotrone Trieste S.C.p.A., Basovizza (Italy)
  3. Politecnico di Milano (Italy); CNR-IFN—Istituto di Fotonica e Nanotecnologie, Milano (Italy)
  4. SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
  5. CNR-ISM—Istituto Struttura della Materia, Trieste (Italy)
  6. Technical University of Denmark, Lyngby (Denmark)
  7. CNR-IOM—Istituto Officina dei Materiali, Trieste (Italy)
  8. CNR-IFN—Istituto di Fotonica e Nanotecnologie, Milano (Italy)
  9. University of Gothenburg (Sweden)
  10. STFC, Daresbury Laboratory, Warrington (United Kingdom)
  11. Politecnico di Milano (Italy)
  12. Kansas State University, Manhattan, KS (United States)
  13. National Research Council of Canada, Ottawa, ON (Canada); University of Ottawa, ON (Canada)
  14. Istituto Madrileño de Estudios Avanzados en Nanociencia (IMDEA-Nanociencia), Madrid (Spain)
  15. Elettra—Sincrotrone Trieste S.C.p.A., Basovizza (Italy); CNR-IOM—Istituto Officina dei Materiali, Trieste (Italy)
The photodissociation dynamics of UV excited CS2 are investigated using time-resolved Auger–Meitner (AM) spectroscopy. AM decay is initiated by inner-shell ionisation with a femtosecond duration x-ray (179.9 eV) probe generated by the FERMI free electron laser. The time-delayed x-ray probe removes an electron from the S(2p) orbital leading to secondary emission of a high energy electron through AM decay. We monitor the electron kinetic energy of the AM emission as a function of pump-probe delay and observe time-dependent changes in the spectrum that correlate with the formation of bound, excited-state CS2 molecules at early times, and CS + S fragments on the picosecond timescale. The results are analysed based on a simplified kinetic scheme that provides a time constant for dissociation of approximately 1.2 ps, in agreement with previous time-resolved x-ray photoelectron spectroscopy measurements (Gabalski, et al 2023 J. Phys. Chem. Lett. 14 7126–7133).
Research Organization:
Kansas State University, Manhattan, KS (United States); SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)
Sponsoring Organization:
Independent Research Fund Denmark-Natural Sciences; Knut and Alice Wallenberg Foundation; Swedish Research Council; USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
AC02-76SF00515; FG02-86ER13491
OSTI ID:
2452851
Alternate ID(s):
OSTI ID: 2447669
OSTI ID: 2574613
OSTI ID: 2919031
Journal Information:
Journal of Physics. B, Atomic, Molecular and Optical Physics, Journal Name: Journal of Physics. B, Atomic, Molecular and Optical Physics Journal Issue: 21 Vol. 57; ISSN 0953-4075; ISSN 1361-6455
Publisher:
IOP PublishingCopyright Statement
Country of Publication:
United States
Language:
English

References (39)

Ionization and fragmentation of OCS and CS2 after photoexcitation around the sulfur 2p edge journal August 1997
A high-resolution magnetic bottle electron spectrometer and its application to a photoelectron–Auger electron coincidence measurement of the L2,3VV Auger decay in CS2 journal January 2014
The Variable Polarization XUV Beamline P04 at PETRA III: Optics, mechanics and their performance
  • Viefhaus, Jens; Scholz, Frank; Deinert, Sascha
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 710 https://doi.org/10.1016/j.nima.2012.10.110
journal May 2013
The seed laser system of the FERMI free-electron laser: design, performance and near future upgrades journal January 2021
Ultrafast Extreme Ultraviolet Photoelectron Spectroscopy of Nonadiabatic Photodissociation of CS 2 from 1 B 2 ( 1 Σ u + ) State: Product Formation via an Intermediate Electronic State journal April 2021
Time-Resolved X-ray Photoelectron Spectroscopy: Ultrafast Dynamics in CS2 Probed at the S 2p Edge journal August 2023
The OCS S L3MM Auger Spectrum and Angular Distributions Studied by Photoelectron−Auger Electron Coincidence Experiments journal August 2009
Ultrafast X-ray Auger probing of photoexcited molecular dynamics journal June 2014
Two-stage seeded soft-X-ray free-electron laser journal October 2013
Time-resolved imaging of purely valence-electron dynamics during a chemical reaction journal April 2011
Acetylacetone photodynamics at a seeded free-electron laser journal January 2018
Following excited-state chemical shifts in molecular ultrafast x-ray photoelectron spectroscopy journal January 2022
X-ray induced Coulomb explosion imaging of transient excited-state structural rearrangements in CS2 journal October 2023
Transient resonant Auger–Meitner spectra of photoexcited thymine journal January 2021
Multichannel photodissociation dynamics in CS2 studied by ultrafast electron diffraction journal January 2022
B21(Σu+1) excited state decay dynamics in CS2 journal December 2006
The ultraviolet photodissociation of CS2: The S(1D2) channel journal January 2012
The direct ultraviolet absorption spectrum of the 1Σ+g→ 1B2(1Σ+u) transition of jet-cooled CS2 journal December 1983
Photofragment spectroscopy of CS 2 at 193 nm: Direct resolution of singlet and triplet channels journal September 1987
A detailed study of the predissociation dynamics of the 1B2(1Σ+u) state of CS2 journal March 1996
A comprehensive study of the vibrationally resolved S 2 p −1 Auger electron spectrum of carbonyl sulfide journal July 2012
Ultrafast predissociation and coherent phenomena in CS2 excited by femtosecond laser pulses at 194–207 nm journal September 1999
Observation of the wavepacket dynamics on the 1 B 2 ( 1 Σ u + ) state of CS 2 by sub-20 fs photoelectron imaging using 159 nm probe pulses journal February 2015
Real-time detection of S(1D2) photofragments produced from the 1B2(1Σu+) state of CS2 by vacuum ultraviolet photoelectron imaging using 133 nm probe pulses journal July 2017
Atomic radiative and radiationless yields for K and L shells journal April 1979
Time resolved detection of the S( 1 D) product of the UV induced dissociation of CS 2 journal January 2021
Transient vibration and product formation of photoexcited CS2 measured by time-resolved x-ray scattering journal October 2022
An x-ray absorption and a normal Auger study of the fine structure in the S2p −1 region of the CS 2 molecule journal April 2009
A modular end-station for atomic, molecular, and cluster science at the low density matter beamline of FERMI@Elettra journal August 2013
Ultrafast dynamics of 2-thiouracil investigated by time-resolved Auger spectroscopy journal January 2020
Optical setup for two-colour experiments at the low density matter beamline of FERMI journal October 2017
Time-resolved inner-shell photoelectron spectroscopy: From a bound molecule to an isolated atom journal April 2018
Mapping the Complete Reaction Path of a Complex Photochemical Reaction journal May 2018
Double Core-Hole Generation in O 2 Molecules Using an X-Ray Free-Electron Laser: Molecular-Frame Photoelectron Angular Distributions journal October 2020
The FERMI free-electron lasers journal April 2015
The Low Density Matter (LDM) beamline at FERMI: optical layout and first commissioning journal April 2015
Multi-resolution electron spectrometer array for future free-electron laser experiments journal August 2021
Time-Resolved Molecular Frame Dynamics of Fixed-in-Space CS2 Molecules journal March 2009
Simultaneous generation of sub-20 fs deep and vacuum ultraviolet pulses in a single filamentation cell and application to time-resolved photoelectron imaging journal September 2013