Comparison of classical, semiclassical and quantum methods in hydrogen broadening of acetylene lines

F. Thibault, S.V. Ivanov, O.G. Buzykin, L. Gomez, M. Dhyne, P. Joubert, M. Lepere

Research output: Contribution to journalArticle

Abstract

Quantum close coupling (CC) calculations of H -broadening coefficients of infrared and isotropic Raman lines of acetylene (C H ) are performed for temperatures between 77 and 2000K. They are used to test three more approximate methods, the quantum coupled states (CS) theory, the semiclassical Robert-Bonamy (RB) formalism and the full classical (FC) model of Gordon. In order to allow a clear and well founded comparison, all the dynamical calculations were performed employing the same ab initio potential energy surface free of any adjustable parameters. It is shown that below room temperature both the coupled states method and full classical method fail at reproducing the close coupling pressure broadening coefficients while above room temperature they are correct and predict comparable accurate values for temperatures greater than about 1000K. The values provided by the RB method are clearly not satisfactory even at the highest temperature examined. However, the temperature dependence of the RB results follows the functional form used for interpolating and extrapolating CC, CS and FC pressure broadening coefficients.
Original languageEnglish
Pages (from-to)1429-1437
Number of pages9
JournalJournal of Quantitative Spectroscopy and Radiative Transfer
Volume112
Issue number9
DOIs
Publication statusPublished - 1 Jun 2011

Fingerprint

Acetylene
acetylene
Hydrogen
pressure broadening
hydrogen
coefficients
room temperature
Temperature
potential energy
formalism
Potential energy surfaces
temperature dependence
temperature
Infrared radiation

Cite this

@article{38759ebc2356401193f159dbba1f90a1,
title = "Comparison of classical, semiclassical and quantum methods in hydrogen broadening of acetylene lines",
abstract = "Quantum close coupling (CC) calculations of H -broadening coefficients of infrared and isotropic Raman lines of acetylene (C H ) are performed for temperatures between 77 and 2000K. They are used to test three more approximate methods, the quantum coupled states (CS) theory, the semiclassical Robert-Bonamy (RB) formalism and the full classical (FC) model of Gordon. In order to allow a clear and well founded comparison, all the dynamical calculations were performed employing the same ab initio potential energy surface free of any adjustable parameters. It is shown that below room temperature both the coupled states method and full classical method fail at reproducing the close coupling pressure broadening coefficients while above room temperature they are correct and predict comparable accurate values for temperatures greater than about 1000K. The values provided by the RB method are clearly not satisfactory even at the highest temperature examined. However, the temperature dependence of the RB results follows the functional form used for interpolating and extrapolating CC, CS and FC pressure broadening coefficients.",
author = "F. Thibault and S.V. Ivanov and O.G. Buzykin and L. Gomez and M. Dhyne and P. Joubert and M. Lepere",
note = "Copyright 2011 Elsevier B.V., All rights reserved.",
year = "2011",
month = "6",
day = "1",
doi = "10.1016/j.jqsrt.2011.02.011",
language = "English",
volume = "112",
pages = "1429--1437",
journal = "Journal of Quantitative Spectroscopy and Radiative Transfer",
issn = "0022-4073",
publisher = "Elsevier Limited",
number = "9",

}

Comparison of classical, semiclassical and quantum methods in hydrogen broadening of acetylene lines. / Thibault, F.; Ivanov, S.V.; Buzykin, O.G.; Gomez, L.; Dhyne, M.; Joubert, P.; Lepere, M.

In: Journal of Quantitative Spectroscopy and Radiative Transfer, Vol. 112, No. 9, 01.06.2011, p. 1429-1437.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Comparison of classical, semiclassical and quantum methods in hydrogen broadening of acetylene lines

AU - Thibault, F.

AU - Ivanov, S.V.

AU - Buzykin, O.G.

AU - Gomez, L.

AU - Dhyne, M.

AU - Joubert, P.

AU - Lepere, M.

N1 - Copyright 2011 Elsevier B.V., All rights reserved.

PY - 2011/6/1

Y1 - 2011/6/1

N2 - Quantum close coupling (CC) calculations of H -broadening coefficients of infrared and isotropic Raman lines of acetylene (C H ) are performed for temperatures between 77 and 2000K. They are used to test three more approximate methods, the quantum coupled states (CS) theory, the semiclassical Robert-Bonamy (RB) formalism and the full classical (FC) model of Gordon. In order to allow a clear and well founded comparison, all the dynamical calculations were performed employing the same ab initio potential energy surface free of any adjustable parameters. It is shown that below room temperature both the coupled states method and full classical method fail at reproducing the close coupling pressure broadening coefficients while above room temperature they are correct and predict comparable accurate values for temperatures greater than about 1000K. The values provided by the RB method are clearly not satisfactory even at the highest temperature examined. However, the temperature dependence of the RB results follows the functional form used for interpolating and extrapolating CC, CS and FC pressure broadening coefficients.

AB - Quantum close coupling (CC) calculations of H -broadening coefficients of infrared and isotropic Raman lines of acetylene (C H ) are performed for temperatures between 77 and 2000K. They are used to test three more approximate methods, the quantum coupled states (CS) theory, the semiclassical Robert-Bonamy (RB) formalism and the full classical (FC) model of Gordon. In order to allow a clear and well founded comparison, all the dynamical calculations were performed employing the same ab initio potential energy surface free of any adjustable parameters. It is shown that below room temperature both the coupled states method and full classical method fail at reproducing the close coupling pressure broadening coefficients while above room temperature they are correct and predict comparable accurate values for temperatures greater than about 1000K. The values provided by the RB method are clearly not satisfactory even at the highest temperature examined. However, the temperature dependence of the RB results follows the functional form used for interpolating and extrapolating CC, CS and FC pressure broadening coefficients.

UR - http://www.scopus.com/inward/record.url?scp=79954609815&partnerID=8YFLogxK

U2 - 10.1016/j.jqsrt.2011.02.011

DO - 10.1016/j.jqsrt.2011.02.011

M3 - Article

AN - SCOPUS:79954609815

VL - 112

SP - 1429

EP - 1437

JO - Journal of Quantitative Spectroscopy and Radiative Transfer

JF - Journal of Quantitative Spectroscopy and Radiative Transfer

SN - 0022-4073

IS - 9

ER -