Transient vibration and product formation of photoexcited CS<sub>2</sub> measured by time-resolved x-ray scattering-Reference-Cited by-同舟云学术

Transient vibration and product formation of photoexcited CS₂ measured by time-resolved x-ray scattering

Published:2022-10-28 Issue:16 Volume:157 Page:164305
ISSN:0021-9606
Container-title:The Journal of Chemical Physics
language:en
Short-container-title:J. Chem. Phys.

Author:

Gabalski Ian¹²^ORCID,Sere Malick¹³^ORCID,Acheson Kyle⁴,Allum Felix¹⁵^ORCID,Boutet Sébastien⁵^ORCID,Dixit Gopal⁶^ORCID,Forbes Ruaridh¹⁵^ORCID,Glownia James M.⁵,Goff Nathan⁷,Hegazy Kareem¹⁸^ORCID,Howard Andrew J.¹²^ORCID,Liang Mengning⁵,Minitti Michael P.⁵^ORCID,Minns Russell S.⁹^ORCID,Natan Adi¹^ORCID,Peard Nolan²^ORCID,Rasmus Weronika O.⁹,Sension Roseanne J.¹⁰^ORCID,Ware Matthew R.¹,Weber Peter M.⁷^ORCID,Werby Nicholas¹⁸^ORCID,Wolf Thomas J. A.¹⁵^ORCID,Kirrander Adam¹¹^ORCID,Bucksbaum Philip H.¹²⁸^ORCID

Affiliation:

1. Stanford PULSE Institute, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

2. Department of Applied Physics, Stanford University, Stanford, California 94305, USA

3. Department of Electrical Engineering, Stanford University, Stanford, California 94305, USA

4. School of Chemistry, University of Edinburgh, Edinburgh EH8 9YL, United Kingdom

5. Linac Coherent Light Source, SLAC National Accelerator Laboratory, Menlo Park, California 94025, USA

6. Department of Physics, Indian Institute of Technology Bombay, Powai, Mumbai 400076, India

7. Department of Chemistry, Brown University, Providence, Rhode Island 02912, USA

8. Department of Physics, Stanford University, Stanford, California 94305, USA

9. School of Chemistry, University of Southampton, Highfield, Southampton SO17 1BJ, United Kingdom

10. Department of Chemistry, University of Michigan, Ann Arbor, Michigan 48109, USA

11. Physical and Theoretical Chemistry Laboratory, Department of Chemistry, University of Oxford, South Parks Road, OX1 3QX Oxford, United Kingdom

Abstract

We have observed details of the internal motion and dissociation channels in photoexcited carbon disulfide (CS2) using time-resolved x-ray scattering (TRXS). Photoexcitation of gas-phase CS2 with a 200 nm laser pulse launches oscillatory bending and stretching motion, leading to dissociation of atomic sulfur in under a picosecond. During the first 300 fs following excitation, we observe significant changes in the vibrational frequency as well as some dissociation of the C–S bond, leading to atomic sulfur in the both 1D and 3P states. Beyond 1400 fs, the dissociation is consistent with primarily 3P atomic sulfur dissociation. This channel-resolved measurement of the dissociation time is based on our analysis of the time-windowed dissociation radial velocity distribution, which is measured using the temporal Fourier transform of the TRXS data aided by a Hough transform that extracts the slopes of linear features in an image. The relative strength of the two dissociation channels reflects both their branching ratio and differences in the spread of their dissociation times. Measuring the time-resolved dissociation radial velocity distribution aids the resolution of discrepancies between models for dissociation proposed by prior photoelectron spectroscopy work.

Funder

Basic Energy Sciences

National Institutes of Health

Leverhulme Trust

National Science Foundation

Engineering and Physical Sciences Research Council

National Defense Science and Engineering Graduate

Familjen Erling-Perssons Stiftelse

Knut Och Alice Wallenbergs Stiftelse

Publisher

AIP Publishing

Subject