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A frequency domain technique is demonstrated which permits the determination of the homogeneous linewidth and relaxation rates of inhomogeneously broadened transitions in crystals, liquids, and glasses. The density-matrix formalism is employed to explain the origins of the intensity-dependent dichroism and birefringence observed in these experiments and to extract the relevant relaxation times. The samples initially studied were liquid solutions of the organic dyes malachite green and 1, 3' -diethyl-2, 2' quinolylthiacarbocyanine iodide. The ground-state recovery times were found to be 1. 20. 1 and 3. 40. 4 ps, respectively, for the two dyes in water solution. The transverse relaxation times were estimated to be less than 0. 02 ps. The present technique is compared to resonant Rayleigh-type three-wave mixing and to time-resolved spectroscopic techniques.
Song et al. (1978) studied this question.