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Journal of Physics B Atomic Molecular and Optical Physics

Mollow splitting of the Na D fluorescence lines in an Ar-filled vapour cell

A R D van Bergen, H. J. van Halewijn, Tj. Hollander, Cornelis Th. J. Alkemade

Published Feb 28, 1988• 1 citation
Publisher

Abstract

The authors have measured time-resolved fluorescence spectra of the Na D lines in an Ar-filled vapour cell, excited by a high-intensity, pulsed dye laser of narrow bandwidth, which was tuned near the D 1 line. The results were compared with a recent theory which also takes into account the polarisation of the laser and the Zeeman degeneracy of the atomic levels. In particular, they predicted and observed a splitting into two components of the D 2 line (whose upper level is populated by mixing collisions), which is a new effect. Because of experimental difficulties, however, they obtained at most a semiquantitative agreement between theory and experiment.

DOI
10.1088/0953-4075/21/4/018

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The authors have measured time-resolved fluorescence spectra of the Na D lines in an Ar-filled vapour cell, excited by a high-intensity, pulsed dye laser of narrow bandwidth, which was tuned near the D 1 line. The results were compared with a recent theory which also takes into account the polarisation of the laser and the Zeeman degeneracy of the atomic levels. In particular, they predicted and observed a splitting into two components of the D 2 line (whose upper level is populated by mixing collisions), which is a new effect. Because of experimental difficulties, however, they obtained at most a semiquantitative agreement between theory and experiment.
Redistribution and depolarisation of light scattered by atoms undergoing collisions outside the impact region of the line profile has been studied experimentally and theoretically. In a cell experiment intensity and linear degree of polarisation of the fluorescence components 32S1/2 to or from 32P1/2,3/2 of Na atoms induced by collisions with Ar buffer gas atoms were measured as functions of the laser frequency omega L. The decrease of polarisation of the D2 component observed when omega L is shifted away from the D2 toward D1 resonance disagrees with calculations on the basis of the factorisation approximation of the theory of redistribution. Using Baylis (1975) potentials for the Na/Ar system, the effect is interpreted in terms of adiabatic coupling of the 32P3/2 electronic angular momentum to the collision axis during 'strong' collisions, giving rise to a greater than average depolarisation.
By tuning a pulsed dye laser through the resonance line of calcium at 422.7 nm the authors have investigated the spectral redistribution of laser radiation by calcium vapour. Two main components were resolved in the side emission from an oven containing calcium vapour and argon buffer gas. These are produced by Rayleigh scattering and by collision-induced fluorescence. The intensity of the Rayleigh component was found to vary as Delta -2 where Delta = omega 21 - omega L is the laser detuning from resonance. In contrast the intensity of the collision-induced fluorescence showed a markedly asymmetric dependence on detuning. Detailed studies of the collision-induced fluorescence have enabled the complete line shape of the calcium resonance line perturbed by argon to be determined. The interpretation of this data in terms of a frequency-dependent collision rate, gamma E ( Delta ), is discussed. This paper also reports calculations of theoretical line profiles using the unified Franck-Condon theory and trial interatomic difference potentials. The comparison of the experimental and theoretical line profiles enables the range of validity of the unified Franck-Condon theory to be assessed and the form of the optimum Ca-Ar difference potential to be selected.
Intensity modulations have been observed in the superradiant signals on the 4 2 P 1/2 -4 2 S 1/2 transitions obtained by pulsed dye laser beam excitation of the 4 2 P 1/2 level in Na vapour. The modulations were interpreted as beats among the frequencies of the electric dipole transitions resulting from the different HFS levels. The HFS splitting both of the upper and the lower levels must be taken into consideration in explaining the observed signals. Preliminary results of the study are reported, in particular the characteristics of the time development and polarisation of the superradiance.
Time-resolved measurements of fluorescence and level populations have been made on barium vapour illuminated by an intense pulse of laser radiation (1 MW cm -2 , 50 ns FWHM) tuned to the resonance transition of Ba I, 6s 2 1 S 0 -6s6p 1 P 1 , at 5535 AA. Barium number densities between 10 13 -10 15 cm -3 were investigated, using a buffer gas of helium at 100 Torr. Fluorescence was measured with two different geometrical arrangements, one allowing partial spatial resolution. In neither case did the observed fluorescence saturate with increasing laser power, although the maximum flux was more than sufficient to burn through the vapour column, as confirmed by transmission measurements. The power loss from the laser beam was found to be compatible with the scattered radiation from the pumped column in the absence of radiation trapping. In contrast to other similar experiments, no significant ionisation was detected (<5%). Time-resolved population measurements by anomalous dispersion on the 6s6p 3 P 2 and 6s5d 1 D 2 metastable levels yielded quenching cross sections for both Ba-Ba and Ba-He collisions, but gave anomalous result for the peak populations. A qualitative explanation of the fluorescence anomaly is proposed on the basis of the AC Stark effect, and it is shown that the same effect can inhibit the onset of stimulated emission to the metastable D levels.
Na atoms in the magnetic field have been selectively excited to each Zeeman sub-level of either the 3p2P1/2 or 3p 2P3/2 state by a tunable dye laser and the Zeeman spectra of the fluorescence from the collisional populated 3p 2P levels have been measured. From the intensities of the Zeeman lines, the selectivity in the collisional transitions between the Zeeman sub-levels of the 3p 2P1/2 and 3p 2P3/2 states has been directly specified. The time evolution of the σ-polarized fluorescence intensity of the Na(3p 2P1/2→ 3s 2S1/2) transition has been measured following the Na(3p 2P3/2â†� 3s 2S1/2) excitation by a σ-polarized short light pulse at H= 129 G. An amplitude modulation was found in the fluorescence from the collisional energy transferred state Na(3p 2P1/2). This is the first observation of quantum beats in collision-induced fluorescence. The frequency of the modulation coincides very well with that of the quantum beats of the resonance fluorescence Na(3p 2P3/2→ 3s 2S1/2), but the phases are opposite. These results are explained by assuming the conservation of coherence during collisional energy transfer.