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Physical Review A

Collisional destruction of four-wave-mixing signals in sodium in the presence of low-pressure buffer gas

Duncan G. Steel, R. A. McFarlane

Published Mar 1, 1983• 15 citations
Publisher

Abstract

We present experimental data showing destruction of degenerate four-wave-mixing signals by collisions at extremely low pressures of added buffer gases (\ensuremath{\sim}100 mtorr). These experiments are performed on the $3s^{2}S_{\frac{1}{2}}(F=2)\ensuremath{-}3p^{2}P_{\frac{3}{2}}(F=3)$ transition of the ${D}_{2}$ line in atomic sodium for which, in the absence of buffer gases, the lower state is not optically pumped to the $3s^{2}S_{\frac{1}{2}}(F=1)$ ground state. However, using a simple rate equation model we are able to qualitatively explain the observed behavior by showing that state-changing collisions have the effect of generating a collision-induced optical pumping. This transfers the $F=2$ ground-state population to the $F=1$ ground state, thus reducing the density of atoms available for generating a signal.

DOI
10.1103/physreva.27.1687

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Annales de Physique•Jan 1, 1985•6 citations
We present experimental data showing destruction of degenerate four-wave-mixing signals by collisions at extremely low pressures of added buffer gases (\ensuremath{\sim}100 mtorr). These experiments are performed on the 3s2S12(F=2)\ensuremath−3p2P32(F=3)3s^{2}S_{\frac{1}{2}}(F=2)\ensuremath{-}3p^{2}P_{\frac{3}{2}}(F=3)3s2S21​​(F=2)\ensuremath−3p2P23​​(F=3) transition of the D2{D}_{2}D2​ line in atomic sodium for which, in the absence of buffer gases, the lower state is not optically pumped to the 3s2S12(F=1)3s^{2}S_{\frac{1}{2}}(F=1)3s2S21​​(F=1) ground state. However, using a simple rate equation model we are able to qualitatively explain the observed behavior by showing that state-changing collisions have the effect of generating a collision-induced optical pumping. This transfers the F=2F=2F=2 ground-state population to the F=1F=1F=1 ground state, thus reducing the density of atoms available for generating a signal.
Optical four-wave mixing resonances in sodium vapor induced by collisions with inert buffer gases (He, Ar, Xe, N2{\mathrm{N}}_{2}N2​) are characterized at high resolution ( 5 MHz) using lasers tuned near the DDD lines of Na. These resonances are interpreted in terms of coherent scattering from a population grating established by collisional absorption of the incident radiation. The roles of homogeneous and inhomogeneous contributions to the resonance line shapes are clarified. The line shapes exhibit structure sharper than the predicted linewidth, that characteristic of the 3P3P3P-to-3S3S3S transition rate. We show that this is caused by collision-induced optical pumping which introduces the ground-state lifetime into the grating relaxation physics. These long-lived gratings are exemplified dramatically by experiments in the presence of N2{\mathrm{N}}_{2}N2​ which collisionally quenches the Na 3P3P3P states. Similar results are obtained in Xe where it is argued that excimer formation with the 3P3P3P states plays a role in the population dynamics. Model calculations of the effects of sodium level degeneracy on the grating dynamics are presented to support these conclusions. Finally we present data illustrating interference between the collision-induced population grating resonances detailed here and collision-induced coherent Raman resonances between Zeeman sublevels of the ground state.
We report a series of measurements of the nearly degenerate four-wave-mixing response in atomic sodium in the presence of a helium buffer gas. The results show the line shape associated with both the ground-state and excited-state dynamics. The line shape evolves as a function of pressure from a dip at a pressure of 0 Torr to a spike at a few Torr due to the presence of collisions. The width of the spike is determined by residual Doppler broadening. At higher pressure (\ensuremath{\ge}10 Torr), the width of the spike is further narrowed below the residual Doppler width. The additional reduction is due to a form of Dicke narrowing associated with the dynamics of the lower- and upper-level excitations. The results are in qualitative agreement with a perturbation solution of the density-matrix equations which include the effects of velocity-changing collisions and state-changing collisions.
Degenerate four-wave mixing (DFWM) in excited atoms is investigated as a probe of the excited-state density produced by collision-assisted transitions. Sodium atoms are excited to the 3P state by absorption of light in the extreme blue wing of the D lines in the presence of He, Ne and Ar perturbers. The rare-gas pressure dependence of the DFWM signals, resonantly enhanced by the 3P-4D transition, is studied to determine the regime where the signals give an unambiguous measure of the excited-state (3P) density. The observed behaviour is compared with a simple model of DFWM in absorbing media. Good qualitative agreement is obtained and the results illustrate the role of absorption, saturation and finite laser bandwidth. The technique allows small excited-state densities ( approximately 10 9 cm -3 ) to be detected with good temporal and spatial resolution.
The influence of molecular collisions on the production of the degenerate four-wave mixing signal in I(2) is presented. Measurements were performed on gaseous molecular iodine, I(2), contained in a glass cell in which pressure, temperature, and species concentration are easily and independently varied. Frequencydoubled outputs from a seeded Nd:YAG laser and an excimer-pumped dye laser were used as excitation sources. We have studied the dependence of signal strength versus buffer gas pressure, with pump intensity as a third parameter. It is evident from our results that, for pump intensities of less than 1 MW/cm(2), the pressure dependence of the signal follows that given by a simple two-level model in the homogeneously broadened regime. In this regime collisional deexcitation becomes significant, leading to changes in saturation intensity. This is evidenced by a reduction in the signal with an increase in buffer gas pressure. This behavior is similar to that seen in laser-induced fluorescence. At higher pump intensities, the signal is seen to increase with pressure; this behavior cannot be described by the simple two-level model.
Collision-enhanced Hanle resonances in the 3 2S1/2^{2}S_{1/2}2S1/2​ electronic ground state of Na atoms have been studied in a phase-conjugate four-wave light-mixing geometry. Narrow resonances in zero magnetic field have been observed at very high inert-buffer-gas pressures, with a width of 21 mG, or less than 10 kHz, full width at half-maximum. The intensity and the width of these resonances has been studied as a function of buffer-gas pressure, of alkali-metal vapor pressure, of detuning from the D1{D}_{1}D1​ and D2{D}_{2}D2​ Na resonances, and of the intensity of the incident light beams. Saturation phenomena and power broadening are observed. The results are explained theoretically in terms of transversely pumped optical gratings. The equivalence of this description with collision-induced coherence gratings in the limit of low light intensities is demonstrated.
First, some historical comments on the Hanle effect and Kastler-type optical pumping are made. Next the recent history of the phenomenon of collision-induced coherences in optical four-wave light mixing experiments is briefly reviewed New experimental results on collision-enhanced Hanle-type resonances in the 3 2S1/2 ground state configuration of Na atoms in a buffer gas at high pressure are presented. The relationship between these optical fourwave experiments and Kastler-type optical pumping is pointed out.