Excitation and relaxation of the asymmetric stretch mode of CO2 in a pulsed glow discharge

B.L.M. Klarenaar, A.S. Morillo-Candas, M. Grofulovic, M.C.M. van de Sanden, R. Engeln, O. Guaitella (Corresponding author)

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Abstract

The excitation and relaxation of the vibrations of CO2; as well as the reduction of CO2 to CO are studied in a pulsed glow discharge. Two diagnostics are employed, being (1) time-resolved in situ Fourier transform nfrared (FTIR) spectroscopy and (2) spatiotemporally resolved in situ rotational Raman spectroscopy. Experiments are conducted within a pressure range of 1.3-6.7 mbar and a current range of 10-50 mA. In the afterglow, the rate of exponential decay from the asymmetric stretch temperature (T3) to the rotational temperature (Trot) is found to be only dependent on Trot, in the conditions under study. The cay rate ρT3-Trot follows the relation ρT3-Trot = 388 s-1 exp(Trot - 273 K)/(154 K). Pressure and varying concentrations of CO and (presumably) atomic oxygen did not show to be of significant influence. In the active part of the discharge the excitation of T3 showed to be positively related to current and negatively to pressure. However, the contribution of current to vibrational excitation is ambiguous: the conversion of CO2 and therefore the fraction of CO in the discharge, is found to be strongly dependent on the current, with a conversion factor of 0.05 to 0.18 for 10 mA to 50 mA, while CO can contribute to the excitation through near-resonant collisions. A clear relation between the elevation of T3 and the dissociation of CO2 could not be confirmed, though conversion peaks are observed in the near afterglow, which motivate future experiments on vibrational ladder-climbing directly after termination of the discharge.
Original languageEnglish
Article number035011
Number of pages14
JournalPlasma Sources Science and Technology
Volume28
Issue number3
DOIs
Publication statusPublished - 12 Mar 2019

Keywords

  • Carbon dioxide plasma
  • Dissociation
  • Fourier transform infrared spectroscopy
  • Glow discharge
  • Raman spectroscopy
  • Vibrational excitation

Cite this

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title = "Excitation and relaxation of the asymmetric stretch mode of CO2 in a pulsed glow discharge",
abstract = "The excitation and relaxation of the vibrations of CO2; as well as the reduction of CO2 to CO are studied in a pulsed glow discharge. Two diagnostics are employed, being (1) time-resolved in situ Fourier transform nfrared (FTIR) spectroscopy and (2) spatiotemporally resolved in situ rotational Raman spectroscopy. Experiments are conducted within a pressure range of 1.3-6.7 mbar and a current range of 10-50 mA. In the afterglow, the rate of exponential decay from the asymmetric stretch temperature (T3) to the rotational temperature (Trot) is found to be only dependent on Trot, in the conditions under study. The cay rate ρT3-Trot follows the relation ρT3-Trot = 388 s-1 exp(Trot - 273 K)/(154 K). Pressure and varying concentrations of CO and (presumably) atomic oxygen did not show to be of significant influence. In the active part of the discharge the excitation of T3 showed to be positively related to current and negatively to pressure. However, the contribution of current to vibrational excitation is ambiguous: the conversion of CO2 and therefore the fraction of CO in the discharge, is found to be strongly dependent on the current, with a conversion factor of 0.05 to 0.18 for 10 mA to 50 mA, while CO can contribute to the excitation through near-resonant collisions. A clear relation between the elevation of T3 and the dissociation of CO2 could not be confirmed, though conversion peaks are observed in the near afterglow, which motivate future experiments on vibrational ladder-climbing directly after termination of the discharge.",
keywords = "Carbon dioxide plasma, Dissociation, Fourier transform infrared spectroscopy, Glow discharge, Raman spectroscopy, Vibrational excitation",
author = "B.L.M. Klarenaar and A.S. Morillo-Candas and M. Grofulovic and {van de Sanden}, M.C.M. and R. Engeln and O. Guaitella",
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Excitation and relaxation of the asymmetric stretch mode of CO2 in a pulsed glow discharge. / Klarenaar, B.L.M.; Morillo-Candas, A.S.; Grofulovic, M.; van de Sanden, M.C.M.; Engeln, R.; Guaitella, O. (Corresponding author).

In: Plasma Sources Science and Technology, Vol. 28, No. 3, 035011, 12.03.2019.

Research output: Contribution to journalArticleAcademicpeer-review

TY - JOUR

T1 - Excitation and relaxation of the asymmetric stretch mode of CO2 in a pulsed glow discharge

AU - Klarenaar, B.L.M.

AU - Morillo-Candas, A.S.

AU - Grofulovic, M.

AU - van de Sanden, M.C.M.

AU - Engeln, R.

AU - Guaitella, O.

PY - 2019/3/12

Y1 - 2019/3/12

N2 - The excitation and relaxation of the vibrations of CO2; as well as the reduction of CO2 to CO are studied in a pulsed glow discharge. Two diagnostics are employed, being (1) time-resolved in situ Fourier transform nfrared (FTIR) spectroscopy and (2) spatiotemporally resolved in situ rotational Raman spectroscopy. Experiments are conducted within a pressure range of 1.3-6.7 mbar and a current range of 10-50 mA. In the afterglow, the rate of exponential decay from the asymmetric stretch temperature (T3) to the rotational temperature (Trot) is found to be only dependent on Trot, in the conditions under study. The cay rate ρT3-Trot follows the relation ρT3-Trot = 388 s-1 exp(Trot - 273 K)/(154 K). Pressure and varying concentrations of CO and (presumably) atomic oxygen did not show to be of significant influence. In the active part of the discharge the excitation of T3 showed to be positively related to current and negatively to pressure. However, the contribution of current to vibrational excitation is ambiguous: the conversion of CO2 and therefore the fraction of CO in the discharge, is found to be strongly dependent on the current, with a conversion factor of 0.05 to 0.18 for 10 mA to 50 mA, while CO can contribute to the excitation through near-resonant collisions. A clear relation between the elevation of T3 and the dissociation of CO2 could not be confirmed, though conversion peaks are observed in the near afterglow, which motivate future experiments on vibrational ladder-climbing directly after termination of the discharge.

AB - The excitation and relaxation of the vibrations of CO2; as well as the reduction of CO2 to CO are studied in a pulsed glow discharge. Two diagnostics are employed, being (1) time-resolved in situ Fourier transform nfrared (FTIR) spectroscopy and (2) spatiotemporally resolved in situ rotational Raman spectroscopy. Experiments are conducted within a pressure range of 1.3-6.7 mbar and a current range of 10-50 mA. In the afterglow, the rate of exponential decay from the asymmetric stretch temperature (T3) to the rotational temperature (Trot) is found to be only dependent on Trot, in the conditions under study. The cay rate ρT3-Trot follows the relation ρT3-Trot = 388 s-1 exp(Trot - 273 K)/(154 K). Pressure and varying concentrations of CO and (presumably) atomic oxygen did not show to be of significant influence. In the active part of the discharge the excitation of T3 showed to be positively related to current and negatively to pressure. However, the contribution of current to vibrational excitation is ambiguous: the conversion of CO2 and therefore the fraction of CO in the discharge, is found to be strongly dependent on the current, with a conversion factor of 0.05 to 0.18 for 10 mA to 50 mA, while CO can contribute to the excitation through near-resonant collisions. A clear relation between the elevation of T3 and the dissociation of CO2 could not be confirmed, though conversion peaks are observed in the near afterglow, which motivate future experiments on vibrational ladder-climbing directly after termination of the discharge.

KW - Carbon dioxide plasma

KW - Dissociation

KW - Fourier transform infrared spectroscopy

KW - Glow discharge

KW - Raman spectroscopy

KW - Vibrational excitation

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U2 - 10.1088/1361-6595/aada5e

DO - 10.1088/1361-6595/aada5e

M3 - Article

VL - 28

JO - Plasma Sources Science and Technology

JF - Plasma Sources Science and Technology

SN - 0963-0252

IS - 3

M1 - 035011

ER -