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Title: Determination of the collisional energy transfer distribution responsible for the collision-induced dissociation of NO 2 with Ar

Abstract

Collisional energy transfer is an essential aspect of chemical reactivity and maintenance of thermal equilibrium. We report the shape (energy-dependence) of the collisional energy transfer probability function for collisions of vibrationally excited NO 2 entrained in a molecular beam and photoexcited to within 40 cm -1 of its dissociation threshold. The internally excited molecules undergo collisions with Ar atoms in a crossed beam apparatus. Dissociative collisions rapidly produce the NO(J) fragment, which is observed by velocity-mapped ion imaging and REMPI techniques. The measured collisional energy transfer function is obtained via energy conservation and is compared with the results of classical trajectory calculations. Good agreement between the theory and experiment is found for collisions that transfer small amounts of energy, but the theory predicts a higher likelihood of energetic collisions than is observed experimentally. We explore possible explanations for this discrepancy in the dynamics of the collision excitation process.

Authors:
 [1];  [1];  [1]
  1. Sandia National Lab. (SNL-CA), Livermore, CA (United States). Combustion Research Facility
Publication Date:
Research Org.:
Sandia National Lab. (SNL-CA), Livermore, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1497644
Alternate Identifier(s):
OSTI ID: 1356260
Report Number(s):
SAND2015-4637J
Journal ID: ISSN 0009-2614; 672344
Grant/Contract Number:  
AC04-94AL85000
Resource Type:
Accepted Manuscript
Journal Name:
Chemical Physics Letters
Additional Journal Information:
Journal Volume: 636; Journal ID: ISSN 0009-2614
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Steill, Jeffrey D., Jasper, Ahren W., and Chandler, David W. Determination of the collisional energy transfer distribution responsible for the collision-induced dissociation of NO2 with Ar. United States: N. p., 2015. Web. doi:10.1016/j.cplett.2015.06.035.
Steill, Jeffrey D., Jasper, Ahren W., & Chandler, David W. Determination of the collisional energy transfer distribution responsible for the collision-induced dissociation of NO2 with Ar. United States. doi:10.1016/j.cplett.2015.06.035.
Steill, Jeffrey D., Jasper, Ahren W., and Chandler, David W. Tue . "Determination of the collisional energy transfer distribution responsible for the collision-induced dissociation of NO2 with Ar". United States. doi:10.1016/j.cplett.2015.06.035. https://www.osti.gov/servlets/purl/1497644.
@article{osti_1497644,
title = {Determination of the collisional energy transfer distribution responsible for the collision-induced dissociation of NO2 with Ar},
author = {Steill, Jeffrey D. and Jasper, Ahren W. and Chandler, David W.},
abstractNote = {Collisional energy transfer is an essential aspect of chemical reactivity and maintenance of thermal equilibrium. We report the shape (energy-dependence) of the collisional energy transfer probability function for collisions of vibrationally excited NO2 entrained in a molecular beam and photoexcited to within 40 cm-1 of its dissociation threshold. The internally excited molecules undergo collisions with Ar atoms in a crossed beam apparatus. Dissociative collisions rapidly produce the NO(J) fragment, which is observed by velocity-mapped ion imaging and REMPI techniques. The measured collisional energy transfer function is obtained via energy conservation and is compared with the results of classical trajectory calculations. Good agreement between the theory and experiment is found for collisions that transfer small amounts of energy, but the theory predicts a higher likelihood of energetic collisions than is observed experimentally. We explore possible explanations for this discrepancy in the dynamics of the collision excitation process.},
doi = {10.1016/j.cplett.2015.06.035},
journal = {Chemical Physics Letters},
number = ,
volume = 636,
place = {United States},
year = {2015},
month = {6}
}

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