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Title: The near-infrared spectrum of ethynyl radical

Abstract

We used transient diode laser absorption spectroscopy to measure three strong vibronic bands in the near infrared spectrum of the C2H, ethynyl, radical not previously observed in the gas phase. The radical was produced by ultraviolet excimer laser photolysis of either acetylene or (1,1,1)-trifluoropropyne in a slowly flowing sample of the precursor diluted in inert gas, and the spectral resolution was Doppler-limited. The character of the upper states was determined from the rotational and fine structure in the observed spectra and assigned by measurement of ground state rotational combination differences. The upper states include a 2Σ+ state at 6696 cm-1, a second 2Σ+ state at 7088 cm-1, and a 2Π state at 7110 cm-1. By comparison with published calculations [R. Tarroni and S. Carter, J. Chem. Phys 119, 12878 (2003); Mol. Phys. 102, 2167 (2004)], the vibronic character of these levels was also assigned. Moreover, the observed states contain both X 2Σ+ and A 2Π electronic characters. Several local rotational level perturbations were observed in the excited states. Kinetic measurements of the time-evolution of the ground state populations following collisional relaxation and reactive loss of the radicals formed in a hot, non-thermal, population distribution were made using some of themore » strong rotational lines observed. Finally, the case of C2H may be a good place to investigate the behavior at intermediate pressures of inert colliders, where the competition between relaxation and reaction can be tuned and observed to compare with master equation models, rather than deliberately suppressed to measure thermal rate constants.« less

Authors:
ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [2]
+ Show Author Affiliations
  1. Brookhaven National Lab. (BNL), Upton, NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1303024
Alternate Identifier(s):
OSTI ID: 1297263
Report Number(s):
BNL-112520-2016-JA
Journal ID: ISSN 0021-9606; JCPSA6; R&D Project: CO006; KC0301020
Grant/Contract Number:  
SC00112704; SC0012704
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 145; Journal Issue: 7; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Le, Anh T., Hall, Gregory E., and Sears, Trevor J. The near-infrared spectrum of ethynyl radical. United States: N. p., 2016. Web. doi:10.1063/1.4961019.
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Le, Anh T., Hall, Gregory E., & Sears, Trevor J. The near-infrared spectrum of ethynyl radical. United States. https://doi.org/10.1063/1.4961019
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Le, Anh T., Hall, Gregory E., and Sears, Trevor J. Wed . "The near-infrared spectrum of ethynyl radical". United States. https://doi.org/10.1063/1.4961019. https://www.osti.gov/servlets/purl/1303024.
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@article{osti_1303024,
title = {The near-infrared spectrum of ethynyl radical},
author = {Le, Anh T. and Hall, Gregory E. and Sears, Trevor J.},
abstractNote = {We used transient diode laser absorption spectroscopy to measure three strong vibronic bands in the near infrared spectrum of the C2H, ethynyl, radical not previously observed in the gas phase. The radical was produced by ultraviolet excimer laser photolysis of either acetylene or (1,1,1)-trifluoropropyne in a slowly flowing sample of the precursor diluted in inert gas, and the spectral resolution was Doppler-limited. The character of the upper states was determined from the rotational and fine structure in the observed spectra and assigned by measurement of ground state rotational combination differences. The upper states include a 2Σ+ state at 6696 cm-1, a second 2Σ+ state at 7088 cm-1, and a 2Π state at 7110 cm-1. By comparison with published calculations [R. Tarroni and S. Carter, J. Chem. Phys 119, 12878 (2003); Mol. Phys. 102, 2167 (2004)], the vibronic character of these levels was also assigned. Moreover, the observed states contain both X 2Σ+ and A 2Π electronic characters. Several local rotational level perturbations were observed in the excited states. Kinetic measurements of the time-evolution of the ground state populations following collisional relaxation and reactive loss of the radicals formed in a hot, non-thermal, population distribution were made using some of the strong rotational lines observed. Finally, the case of C2H may be a good place to investigate the behavior at intermediate pressures of inert colliders, where the competition between relaxation and reaction can be tuned and observed to compare with master equation models, rather than deliberately suppressed to measure thermal rate constants.},
doi = {10.1063/1.4961019},
journal = {Journal of Chemical Physics},
number = 7,
volume = 145,
place = {United States},
year = {Wed Aug 17 00:00:00 EDT 2016},
month = {Wed Aug 17 00:00:00 EDT 2016}
}
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