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Abstract: The pure rotational Raman linewidths of the symmetric‐top molecule C2H6 are determined from a time‐resolved femtosecond experiment at room temperature and moderate pressure in a pump‐probe scheme. After excitation by a strong 100 fs‐duration nonresonant near infrared pump pulse, the molecular sample exhibits periodic post‐pulse alignment revivals that produce an anisotropic angular distribution of the molecular axis. Such molecular motion induces in turn a time‐dependent optical birefringence, which can be probed using a weak time‐delayed probe pulse. The Fourier transform of the temporal signal, recorded over a wide time delay range (several hundred picoseconds) for high frequency resolution, is directly related to the rotational Raman spectrum of ethane molecules. The Raman lines are analyzed with a frequency lineshape taking into account the collisional relaxation and the apparatus function. The linewidths are measured for rotational quantum numbers J=3 to J=30 in the pressure range 0.69–1.06 bar. A decrease of the collisional broadening coefficient is observed as J increases. These first measurements of pure rotational Raman linewidths of ethane are compared with previously reported infrared and far‐infrared values. [ABSTRACT FROM AUTHOR]

In this paper, laser-induced field-free alignment of CO2 in mixtures with Ar is investigated under dissipative conditions (up to 15 bars) at room temperature. The degree of alignment is temporally monitored by a polarization spectroscopy technique, where a weak probe pulse measures the transient birefringence resulting from the alignment. The data are analyzed with a quantum mechanical density matrix formalism using properly J-dependent and M-dependent state-to-state transfer rates, which was previously successfully tested on pure CO2 and CO2-He mixtures. The same consistency is obtained between experiments and calculations, in particular the decay times of both the transient revivals and the permanent component of the alignment are accurately predicted by the model. Copyright © 2015 John Wiley & Sons, Ltd. [ABSTRACT FROM AUTHOR]

Abstract: The pure rotational Raman linewidths of the symmetric‐top molecule C2H6 are determined from a time‐resolved femtosecond experiment at room temperature and moderate pressure in a pump‐probe scheme. After excitation by a strong 100 fs‐duration nonresonant near infrared pump pulse, the molecular sample exhibits periodic post‐pulse alignment revivals that produce an anisotropic angular distribution of the molecular axis. Such molecular motion induces in turn a time‐dependent optical birefringence, which can be probed using a weak time‐delayed probe pulse. The Fourier transform of the temporal signal, recorded over a wide time delay range (several hundred picoseconds) for high frequency resolution, is directly related to the rotational Raman spectrum of ethane molecules. The Raman lines are analyzed with a frequency lineshape taking into account the collisional relaxation and the apparatus function. The linewidths are measured for rotational quantum numbers J=3 to J=30 in the pressure range 0.69–1.06 bar. A decrease of the collisional broadening coefficient is observed as J increases. These first measurements of pure rotational Raman linewidths of ethane are compared with previously reported infrared and far‐infrared values. [ABSTRACT FROM AUTHOR]