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A 193-nm-laser photofragmentation time-of-flight mass spectrometric study of dimethylsulfoxide

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.473025· OSTI ID:435117
; ; ;  [1]; ;  [2]
  1. Ames Laboratory, USDOE, and Department of Chemistry, Iowa State University, Ames, Iowa 50011 (United States)
  2. Department of Chemistry, Iowa State University, Ames, Iowa 50011 (United States)

The photodissociation of dimethylsulfoxide [(CH{sub 3}){sub 2}SO] at 193.3 nm has been investigated using the molecular beam time-of-flight (TOF) mass spectrometric technique. In addition to CH{sub 3} and SO, CH{sub 3}SO is also observed as a stable primary product, indicating that CH{sub 3}SO+CH{sub 3} is an important product channel for the 193.3 nm photodissociation of (CH{sub 3}){sub 2}SO. The analysis of the TOF data provides evidence that SO is formed via a stepwise mechanism: (CH{sub 3}){sub 2}SO+h{nu} (193.3 nm){r_arrow}CH{sub 3}SO+CH{sub 3}{r_arrow}2CH{sub 3}+SO. The analysis also indicates that {approx}53{percent} of the primary CH{sub 3}SO radicals undergo further dissociation to produce CH{sub 3}+SO, yielding a quantum yield of {approx}1.53 for CH{sub 3}. Within the sensitivity of our experiment, the product channel of CH{sub 3}SCH{sub 3}+O is not found. The angular distribution for the formation of CH{sub 3}SO+CH{sub 3} is found to be isotropic, an observation consistent with a predissociation mechanism, in which the dissociation of photoexcited (CH{sub 3}){sub 2}SO is slow compared to its rotational period. The energetics for selected dissociation reactions of (CH{sub 3}){sub 2}SO have also been investigated by {ital ab initio} calculations at the G2(MP2) level of theory. The experimental dissociation energy at 0 K (53{plus_minus}2 kcal/mol) for the CH{sub 3}{endash}SOCH{sub 3} bond obtained here is in excellent agreement with the theoretical prediction of 52.6 kcal/mol. {copyright} {ital 1997 American Institute of Physics.}

Research Organization:
Ames National Laboratory
DOE Contract Number:
W-7405-ENG-82
OSTI ID:
435117
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 1 Vol. 106; ISSN 0021-9606; ISSN JCPSA6
Country of Publication:
United States
Language:
English