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1.
Using a high resolution Raman spectrometer, we have measured Ar-broadening coefficients in the ν2Q branch of C2H2 for 22 lines at 295 K, 20 lines at 174 K, and 16 lines at 134 K. These lines with J values ranging from 1 to 23 are located in the spectral range 1970.9-1974.3 cm−1. The collisional widths are obtained by fitting each spectral line with a Rautian profile. The resulting broadening coefficients are compared with theoretical values arising from close coupling and coupled states calculations. A satisfactory agreement is obtained at room as well as at low temperatures, especially for odd J lines. By comparing broadening coefficients at 295, 174, and 134 K from a simple power law, the temperature dependence of these broadenings has been determined both experimentally, and theoretically. 相似文献
2.
Jean-Marcel Colmont François Rohart Jean-Pierre Bouanich 《Journal of Molecular Spectroscopy》2006,238(1):98-107
Extensive experiments on the K = 3 component of the J = 12-11 rotational transition of acetonitrile CH3C14N, located near 220.7 GHz, were performed at different temperatures in the range 235-350 K. They allow determining the N2-, H2-, and He-broadening coefficients, as well as their temperature dependences. More specific measurements on all the K-components of the involved transition perturbed by N2 at 303 K allow to point out a clear decreasing of the broadening coefficient with increasing K. Narrowing effects are clearly observed, and experimental lines were analysed both with Voigt and speed dependent Voigt profiles; but no exhaustive lineshape study was carried out. All the experimental parameters are compared with results derived from a semiclassical calculation of collisional interactions, including electrostatic, induction, and dispersion energy contributions. 相似文献
3.
Muriel Lepère Ghislain Blanquet Jacques Walrand Jean-Pierre Bouanich 《Journal of Molecular Spectroscopy》1996,180(2):218-226
Infrared absolute line intensities of the ν6band of CH3F have been measured around 8.5 μm using a diode-laser spectrometer. These line strengths were obtained by the equivalent width method and, for 13 lines, by fitting a Rautian profile to the measured shape of the lines. From these results, we have deduced the vibrational band strength to beS0v= 9.66 ± 0.13 cm−2atm−1at 296 K and the first Herman–Wallis factors. 相似文献
4.
N2-broadening coefficients have been measured for 41 transitions of PH3 at −100 °C in the QR branch of the ν2 band and the PP, RP, and SP branches of the ν4 band, using a tunable diode-laser spectrometer. The recorded lines with J values ranging from 1 to 13 and K from 0 to 10 are located between 1026 and 1093 cm−1. The collisional widths are determined by fitting each spectral line with a Voigt profile, a Rautian profile, and a speed-dependent Rautian profile. The latter models provide larger broadening coefficients than the Voigt model. These coefficients have also been calculated on the basis of a semiclassical model of interacting linear molecules by considering an atom-atom Lennard-Jones potential in addition to the electrostatic contributions. By comparing broadening coefficients at room and low temperatures, the temperature dependence of these broadenings has been determined both experimentally and theoretically. 相似文献
5.
Christophe Lerot Ghislain Blanquet Jean-Pierre Bouanich 《Journal of Molecular Spectroscopy》2003,219(2):329-334
Using a diode-laser spectrometer, we have measured H2-broadening coefficients of CH3D at low temperatures (153.5, 183.5, and 223.5 K) for four lines in the ν3 band. The collisional widths are obtained by fitting each absorption line with three lineshape models: the Voigt, Rautian, and Galatry profiles. The broadening coefficients are also calculated on the basis of a semiclassical model of interacting linear molecules by considering an atom-atom Lennard-Jones potential in addition to electrostatic contributions. By comparing the broadening coefficients at room and low temperatures the temperature dependence of these broadenings has been determined both experimentally and theoretically. 相似文献
6.
J.P. Bouanich A. Predoi-Cross R.L. Sams C.P. Rinsland V. Malathy Devi 《Journal of Molecular Spectroscopy》2005,231(1):85-95
A semiclassical theory based upon the Robert-Bonamy formalism has been developed to explain the experimental measurements of self-broadening, self-induced pressure shift coefficients in the ν1,ν2, 2ν2 bands of H12C14N and the 2ν1 band of H13C14N, as well as the temperature dependences of these parameters with special emphasis on the ν2 band. Our calculations include only electrostatic interactions and neglect the vibrational dependence of the isotropic part of the intermolecular potential, which probably has a weak contribution to the HCN self-shifts for the bands investigated in this study. The agreement between theory and measurements is good in the cases of self-broadening coefficients and their variation with temperature, as well as the self-shift coefficients determined at room temperature. However, the observed temperature dependence of self-shift coefficients in the ν2 band is different from that derived theoretically. 相似文献
7.
N2-broadening coefficients are measured for 61 transitions of PH3 in the QR branch of the ν2 band and the PP, RP, SP, and PQ branches of the ν4 band, using a tunable diode-laser spectrometer. The recorded lines with J values ranging from 1 to 16 and K from 0 to 11 are located between 1008 and 1106 cm−1. The collisional widths are determined by fitting each spectral line with a Voigt profile, a Rautian profile, and a speed-dependent Rautian profile. The latter models provide larger broadening coefficients than the Voigt model. These coefficients have also been calculated on the basis of a semiclassical model of interacting linear molecules by considering an atom-atom Lennard-Jones potential in addition to the electrostatic contributions. The theoretical results are in good agreement with the experimental data and reproduce the J dependence of the broadenings, but their decrease at high J values is overestimated for the QR (J, K) transitions. 相似文献
8.
For the purpose of atmospheric applications, we have measured N2- and O2-induced broadenings and shapes of rotational lines of N2O in the 235-350 K temperature range, precisely the J=8←7, J=22←21, and J=23←22 lines, located near 201, 552, and 577 GHz, respectively. The analysis of experimental lineshapes shows up significant deviations from the Voigt profile, which are characteristic of line narrowing processes. In a first step, the Voigt profile was considered for the determination of pressure broadening parameters and of their temperature dependencies. Results are in good agreement with the dependence from rotational quantum number previously observed for other rotational and rovibrational lines. They are well explained by calculations based on a semiclassical formalism that includes the atom-atom Lennard-Jones potential in addition to electrostatic interactions up to hexadecapolar contributions. In a second step, observed lineshapes were analyzed by using the Galatry profile and a speed-dependent Voigt profile. The nonlinear pressure behavior observed for the diffusion rate β involved in the Galatry profile leads to rule out the possible role of velocity/speed changing collisions, and to infer that discrepancies from the Voigt profile result from the dependence of relaxation rates on molecular speeds. This interpretation is supported by the comparison of optical and kinetic radii and confirmed by theoretical calculations of relaxation rates. Finally, it can be claimed that, for the N2O-N2 and N2O-O2 systems, deviations from the Voigt profile are explained by a speed-dependent Voigt profile. 相似文献
9.
In this study we report the first measurements of the pressure-induced lineshift coefficients due to Ar, He, O2, and N2 for 22 rovibrational lines from P(53) to R(53), belonging to the 2ν3 band of 16O12C32S at 4100 cm−1. The lineshift results were obtained from the simultaneous record of the pressure-broadened and pure low-pressure OCS lines, using a tunable difference-frequency laser spectrometer. For four lines of the 2ν3 band we also report Ar-, He-, O2-, and N2-broadening coefficients by fitting Voigt and Rautian profiles to the measured shapes of these lines. The broadening and shift coefficients are compared to the results of theoretical calculations based on the semiclassical Robert–Bonamy formalism and two different isotropic and anisotropic intermolecular potentials. For OCS–Ar we also consider the Smith–Giraud–Cooper model including all orders of the interaction within the peaking approximation. In all cases, the calculated broadening coefficients are in reasonable agreement with the experimental data. By considering adjustable parameters for the vibrational dependence of the isotropic potential, the general trends of the lineshifts with J can be roughly predicted, except at low J values where an asymmetry behavior for P and R branches is generally observed. 相似文献
10.
Ar-broadening coefficients have been measured in the P- and R-branches of the ν5 fundamental band of C2H2 for 30 lines at room temperature and 8 lines at −100 °C, using a tunable diode-laser spectrometer. These lines with J values ranging from 2 to 27 are located in the spectral range 665-795 cm−1. The collisional widths are obtained by fitting each absorption line with three lineshape models: the Voigt profile, the Rautian profile accounting for the Dicke narrowing effect, and a general Rautian profile including the absorber speed-dependent collisional broadening. The latter model provides significantly larger broadening coefficients than the Voigt model. These coefficients are also calculated from a semiclassical theory performed by using a simple intermolecular potential with two adjustable parameters. Finally, the temperature dependence of the broadening coefficients has been determined both experimentally and theoretically. 相似文献