Advanced

Collisional broadening and spectral shapes of absorption lines of free and nanopore-confined O-2 gas

Hartmann, J. -M.; Sironneau, V.; Boulet, C.; Svensson, T.; Hodges, J. T. and Xu, Can LU (2013) In Physical Review A (Atomic, Molecular and Optical Physics) 87(3).
Abstract
This paper presents fully ab initio calculations of the broadenings and spectral shapes of O-2 infrared absorption lines in a free gas and when confined in nanoporous media. These calculations are performed, without use of any adjusted parameter, using a recently proposed approach [Phys. Rev. A 87, 013403 (2013)] that is based on requantized classical molecular-dynamics simulations. This involves studying the time evolutions of the translational and rotational motions of large numbers of molecules taking molecule-molecule and molecule-surface collisions into account through realistic interaction potentials. These simulations enable predictions of dipole autocorrelation functions whose Fourier-Laplace transforms yield the associated... (More)
This paper presents fully ab initio calculations of the broadenings and spectral shapes of O-2 infrared absorption lines in a free gas and when confined in nanoporous media. These calculations are performed, without use of any adjusted parameter, using a recently proposed approach [Phys. Rev. A 87, 013403 (2013)] that is based on requantized classical molecular-dynamics simulations. This involves studying the time evolutions of the translational and rotational motions of large numbers of molecules taking molecule-molecule and molecule-surface collisions into account through realistic interaction potentials. These simulations enable predictions of dipole autocorrelation functions whose Fourier-Laplace transforms yield the associated spectra. Comparisons are then made with broadening coefficients and line shapes provided by new and previous experiments. The good agreement between calculated and measured results confirms the veracity of the proposed model for a free gas and shows that the effects of confinement, which induce significant modifications to the line shapes, are correctly predicted. The need for improved characterization of the shape and size of pores in random nanoporous media is highlighted. DOI: 10.1103/PhysRevA.87.032510 (Less)
Please use this url to cite or link to this publication:
author
organization
publishing date
type
Contribution to journal
publication status
published
subject
in
Physical Review A (Atomic, Molecular and Optical Physics)
volume
87
issue
3
publisher
American Physical Society
external identifiers
  • wos:000316319300006
  • scopus:84875316520
ISSN
1050-2947
DOI
10.1103/PhysRevA.87.032510
language
English
LU publication?
yes
id
619e38ce-a6ee-42d0-9c11-7920890ae34d (old id 3765082)
date added to LUP
2013-05-20 09:56:59
date last changed
2019-03-12 01:31:54
@article{619e38ce-a6ee-42d0-9c11-7920890ae34d,
  abstract     = {This paper presents fully ab initio calculations of the broadenings and spectral shapes of O-2 infrared absorption lines in a free gas and when confined in nanoporous media. These calculations are performed, without use of any adjusted parameter, using a recently proposed approach [Phys. Rev. A 87, 013403 (2013)] that is based on requantized classical molecular-dynamics simulations. This involves studying the time evolutions of the translational and rotational motions of large numbers of molecules taking molecule-molecule and molecule-surface collisions into account through realistic interaction potentials. These simulations enable predictions of dipole autocorrelation functions whose Fourier-Laplace transforms yield the associated spectra. Comparisons are then made with broadening coefficients and line shapes provided by new and previous experiments. The good agreement between calculated and measured results confirms the veracity of the proposed model for a free gas and shows that the effects of confinement, which induce significant modifications to the line shapes, are correctly predicted. The need for improved characterization of the shape and size of pores in random nanoporous media is highlighted. DOI: 10.1103/PhysRevA.87.032510},
  articleno    = {032510},
  author       = {Hartmann, J. -M. and Sironneau, V. and Boulet, C. and Svensson, T. and Hodges, J. T. and Xu, Can},
  issn         = {1050-2947},
  language     = {eng},
  number       = {3},
  publisher    = {American Physical Society},
  series       = {Physical Review A (Atomic, Molecular and Optical Physics)},
  title        = {Collisional broadening and spectral shapes of absorption lines of free and nanopore-confined O-2 gas},
  url          = {http://dx.doi.org/10.1103/PhysRevA.87.032510},
  volume       = {87},
  year         = {2013},
}