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Collisional and saturation effects in multiphoton processes in the field of two pumps

G. S. Agarwal, N. Nayak

Published Jan 1, 1986• 0 citations
OpenAlex

Abstract

The nonlinear response of a two-level system interacting with two pump beams of different frequencies is studied with a view to examine several recent experiments on nonlinear mixing of high orders, instabilities in homogeneously broadened lasers, and holes in homogeneous lines. Such a nonlinear response is calculated with use of the continued fractions given in our earlier work [J.Opt. Soc. Am. 81, 164 (1984)]. Saturation effects lead to the appearance of many structures at submultiples of the Rabi frequency. The origin of these subharmonics in nonlinear-response functions is explained. It is shown that collisions not only lead to hole burning at the line center for weak fields but can also lead in moderate fields to the appearance of structures at subharmonics of the Rabi frequency. Existence of collision-induced coherences similar to those in four-wave mixing is shown in six-wave mixing. Exact results for the degenerate nonlinear mixing of arbitrary order are presented for arbitrary values of field strengths. Saturating fields create holes at the line center of such nonlinear mixing signals. Gain profiles of two modes symmetrically displaced from line center are also given. Numerical results, with complete account of saturation and collisions, for a variety of nonlinear-response functions are presented.

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Journal of the Optical Society of America B•Apr 1, 1984•86 citations
The nonlinear response of a two-level system interacting with two pump beams of different frequencies is studied with a view to examine several recent experiments on nonlinear mixing of high orders, instabilities in homogeneously broadened lasers, and holes in homogeneous lines. Such a nonlinear response is calculated with use of the continued fractions given in our earlier work [J.Opt. Soc. Am. 81, 164 (1984)]. Saturation effects lead to the appearance of many structures at submultiples of the Rabi frequency. The origin of these subharmonics in nonlinear-response functions is explained. It is shown that collisions not only lead to hole burning at the line center for weak fields but can also lead in moderate fields to the appearance of structures at subharmonics of the Rabi frequency. Existence of collision-induced coherences similar to those in four-wave mixing is shown in six-wave mixing. Exact results for the degenerate nonlinear mixing of arbitrary order are presented for arbitrary values of field strengths. Saturating fields create holes at the line center of such nonlinear mixing signals. Gain profiles of two modes symmetrically displaced from line center are also given. Numerical results, with complete account of saturation and collisions, for a variety of nonlinear-response functions are presented.
The nonlinear response of a two-level system interacting with two pump beams of different frequencies is studied with a view to examine several recent experiments on nonlinear mixing of high orders, instabilities in homogeneously broadened lasers, and holes in homogeneous lines. Such a nonlinear response is calculated with use of the continued fractions given in our earlier work [J. Opt. Soc. Am. B1, 164 (1984)]. Saturation effects lead to the appearance of many structures at submultiples of the Rabi frequency. The origin of these subharmonics in nonlinear-response functions is explained. It is shown that collisions not only lead to hole burning at the line center for weak fields but can also lead in moderate fields to the appearance of structures at subharmonics of the Rabi frequency. Existence of collision-induced coherences similar to those in four-wave mixing is shown in six-wave mixing. Exact results for the degenerate nonlinear mixing of arbitrary order are presented for arbitrary values of field strengths. Saturating fields create holes at the line center of such nonlinear mixing signals. Gain profiles of two modes symmetrically displaced from line center are also given. Numerical results, with complete account of saturation and collisions, for a variety of nonlinear-response functions are presented.
A very large number of physical phenomena in the resonant interaction of atomic-molecular systems with the radiation fields can be studied by treating the atomic system as a two level system and by examining its response to the applied fields. Various perturbative results are well known. A number of recent experimental works require the knowledge of the nonperturbative response functions, when both the applied fields are strong. These include a variety of experiments on instabilities(1) in lasers involving the switching from a single mode to for example two mode operation. Similarly recent nonlinear mixing experiments, where not only four wave mixing but also higher mixing in saturating fields has been studied. Pump probe experiments have also been repeated with probes whose intensity could be large. The purpose of this paper is to formulate the general theory and use it to understand the experiments. The formulation we present is also well suited for studying the effect of collisions. Details of various collisional induced coherences in fourwave and six wave mixing etc. can be studied.
We present in this paper a theory of the saturation effects in degenerate four-wave mixing which makes use of the dressed-atom method. We mainly study the case of a Doppler-broadened line, but several results can be applied to the case of nearly degenerate four-wave mixing for a Doppler-free medium. We show that a close relationship does exist between the two problems : the generated beam is mainly created when the detuning between two incident beams is equal to the Rabi frequency. In the degenerate case, this condition is fulfilled by two velocity groups because of the Doppler shift. We analytically calculate the lineshapes for two-level atoms in the case of forward saturation (the intense pump beam propagates in the same direction than the probe beam) and in the case of backward saturation (the intense pump beam and the probe beam propagate in opposite directions). We also study collisional effects and the influence of the intensity of the weak pump beam when perturbation theory can no longer be applied.
Polarization and Rayleigh type optical mixing spectra of a homogeneously and inhomogeneously broadened two-level system are calculated. We show that the nonlinear signal has contributions from the population pulsation and saturation effect. In the homogeneous system these effects can induce an asymmetric spectrum when the probe frequency is different from the resonant value. In the inhomogeneous system the spectral response is always symmetric independent of the probe frequency value. Line saturation and dynamic stark splitting are substantially reduced in the inhomogeneous case. The mentioned differences can be used to identify the type of broadening of a given spectral line.
Two-photon transitions have provided the basis for numerous useful nonlinear interactions with radiation. In this paper we calculate the absorption and coupling coefficients for one-, two-, and three-wave mixing in two-photon homogeneously broadened media. The resulting field equations form the basis for understanding saturation spectroscopy, phase conjugation,1 and single-mode instabilities2 in lasers and optical bistability in two-photon media. We assume that the wave frequencies are not resonant with any intermediate state j and that the probe and conjugate waves cannot saturate the two-photon transition. This allows us to use the two-photon two-level model and to transfer much of our knowledge of the one-photon two-level systems to the two-photon case. Two major differences occur between the two models. First, dynamic Stark shifts of the active levels play an important role in generating asymmetric spectra and nonzero dispersion (≃ω s T1) at line center. Second, high pump intensities do not bleach the absorption coefficient at the Rabi sidebands.
The dynamical behavior of a two-level atom under the influence of two intense pump beams is examined. Exact equations for the nonlinear susceptibilities to all orders in the field strengths are derived. Numerical results for the nonlinear susceptibilities giving the absorption of the radiation from either of the pump beams and the generation of the four-wave mixing signal are given. The susceptibility for four-wave mixing, in addition to showing various saturation peaks, shows a peak at ω1 = ω2 even in the case of radiative relaxation. Higher-order multiphoton peaks in the absorption spectra are found to be extremely sensitive to the temporal fluctuations in the pumps.