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Journal of the Optical Society of America B

Ultranarrow optical resonances and measurements of relaxation rates using resonant four-wave mixing

Duncan G. Steel, Stephen Colby Rand, J. Remilard

Published Feb 1, 1986• 0 citations
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This paper presents perturbation calculations using the density matrix to describe the nearly degenerate four-wave-mixing spectral response in resonant systems subject to state-specific reservoir coupling. The calculations provide physical insight into the origin of narrow resonances observed in recent experimental work in atomic sodium and ultranarrow resonances in crystals. The calculations are for systems which are homogeneously broadened as well as systems which are inhomogeneously broadened due to velocity effects or random crystal fields. The calculations show that it is possible to eliminate the effects of either kind of broadening and measure the decay rate of the dipole coherence as well as the decay rates of both states of the transition. Furthermore, the calculations indicate that the method of cross-correlated optical fields which was used to eliminate the effects of laser jitter in longitudinal relaxation rate measurements could be extended to the measurements of slow dephasing rates in crystals.
We apply two-photon resonant nondegenerate four-wave mixing with a resonant intermediate state to the observation of the broadening and shifting of the barium Rydberg level 6s24d 1 D 2 by collision with argon. The collision broadening and shifting cross sections are measured. This technique is purely optical, and can investigate the pressure dependence of the transverse relaxation rate Γ 21 between the Rydberg state and an intermediate state, as well as the transverse relaxation rate Γ 20 between the Rydberg state and the ground state.