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Physical Review A

New component in degenerate four-wave mixing of optical pulses in sodium vapor

Salim N. Jabr, L. K. Lam, R. W. Hellwarth

Published Dec 1, 1981• 26 citations
Publisher

Abstract

We have observed a new component in the signals produced by degenerate four-wave mixing of 5-nsec optical pulses by the $D$-line resonances of sodium vapor. This component is comparable in intensity to that previously observed from a grating pattern of excited sodium atoms, but arises rather from a grating of coherently aligned (but not optically pumped) ground-state atoms. This component exists when there are no spatial intensity beats between input waves.

DOI
10.1103/physreva.24.3264

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We have observed a new component in the signals produced by degenerate four-wave mixing of 5-nsec optical pulses by the DDD-line resonances of sodium vapor. This component is comparable in intensity to that previously observed from a grating pattern of excited sodium atoms, but arises rather from a grating of coherently aligned (but not optically pumped) ground-state atoms. This component exists when there are no spatial intensity beats between input waves.
In femtosecond degenerate four-wave mixing experiments in sodium vapor, quantum beats are observed at the wavelength of the third harmonic when the fundamental beams are three-photon resonant. The period of beating, which corresponds to fine structure energy-level splitting, does not change with the atomic number density, buffer gas pressure, or laser intensity. Surprisingly, the third-harmonic signal is observed only at negative time delays for the transient grating pulse sequence. We relate this to the well-known interference effect between excitation pathways involving the fundamental and the third-harmonic fields, which leaves atoms virtually unexcited and prevents formation of population grating.
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.
Degenerate four-wave mixing (DFWM) line shapes are investigated in sodium vapor near the D(2) resonance line using nearly Fourier-transform-limited pulses. At low pump intensities sub-Doppler resolution is obtained. When the Rabi frequency associated with the pump intensity becomes comparable with the ground-state hyperfine frequency separation of sodium, each component of the double-peaked DFWM spectrum splits further into two components. An adiabatic-following model explains the near-resonant intensity dependence of the DFWM signal. A qualitative explanation of the observed splitting is also given.
Degenerate four-wave mixing in sodium vapor is investigated using a flashlamp-pumped dye laser synchronized on a cw dye laser. At low atomic density, the reflectivity versus the pump intensity and the line shapes are in good agreement with theoretical predictions in the case of both plane waves and Gaussian beams. At high atomic density, reflectivities much higher than unity have been observed. The influence of the pump imbalance has been studied as well as the deformation of the wave front of the conjugated beam introduced by the pump beams. In the high-atomic-density case, the theoretical problem is more complex, and our experimental results exhibit only qualitative agreement with theory.
Degenerate four-wave mixing in dense sodium vapor under conditions of strong pressure-induced Zeeman pumping is investigated. Thermal diffusion and its interplay with the Zeeman light shift are found to be responsible for the generation of a grating mechanism that is not sensitive to thermal washout. The effect can be observed experimentally after eliminating the influence of radiation trapping by the use of nitrogen as a buffer gas. Under these conditions large nonlinearities are produced which also influence the propagation of the signal wave via collision-aided circular birefringence.