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Physical Review A

Nonperturbative analysis of four-wave mixing in a four-level system with three strong fields

David A. Coppeta, Paul L. Kelley, P. J. Harshman, T. Kenneth Gustafson

Published Feb 1, 1996• 9 citations
Publisher

Abstract

Radiative renormalization is used to obtain an exact steady-state solution of a four-level system coupled by three arbitrarily strong, near-resonant, monochromatic fields. The four-wave mixing and absorption terms are given for a weak fourth field. The results demonstrate the effects of optically induced energy-level mixing and shifting, and population redistribution. \textcopyright{} 1996 The American Physical Society.

DOI
10.1103/physreva.53.925

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Radiative renormalization is used to obtain an exact steady-state solution of a four-level system coupled by three arbitrarily strong, near-resonant, monochromatic fields. The four-wave mixing and absorption terms are given for a weak fourth field. The results demonstrate the effects of optically induced energy-level mixing and shifting, and population redistribution. \textcopyright{} 1996 The American Physical Society.
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A nonperturbative semiclassical theory is presented for the treatment of four-wave mixing (FWM) in a four-level system. This treatment is based on a transformation to a generalized rotating frame followed by a numerical diagonalization of the resulting time-independent Hamiltonian. For strong fields, all resonant frequencies are shifted from the atomic (molecular) frequencies. Lines are split up in a way similar to the ac Stark effect for a two-level system, and for even stronger fields, the effect of stirring is observed for the first time in four-wave mixing. In addition, a new extra resonance appears which is induced by the saturating field. This field-induced resonance is the new member in the family of extra resonances (pressure induced, or stochastic fluctuation induced), and it should be observed whenever saturating fields interact with a multilevel atomic or molecular system.
An explicit solution is obtained for the four-wave frequency mixing ${\ensuremath{\omega}}_{d}={\ensuremath{\omega}}_{a}\ensuremath{-}{\ensuremath{\omega}}_{b}+{\ensuremath{\omega}}_{c}$ of two strong fields a and c and two weak fields b and d in a four-level system with large Doppler broadening in collinear geometry, where the frequencies of weak fields are nearly equal, ${\ensuremath{\omega}}_{b}\ensuremath{\simeq}{\ensuremath{\omega}}_{d},$ and the medium is optically thin. Without weak fields there are two independent two-level systems. A pair of weak fields probes two other allowed transitions. A peak of the mixing coefficient as a function of intensity is found around an equal Rabi splitting of both two-level systems. The effect is based on a resonance between two closed cycles of four-wave mixing via different dressed states. Three, four, or six peaks are predicted in the dependence of the mixing coefficient on the frequency of the weak field; two of them are a consequence of averaging over velocities. The model allows an interpretation of the dependence of the output wave power on the intensity and detuning in recent experiments on frequency mixing in sodium vapor.
The effect of electromagnetically induced transparency in resonant four-wave-mixing schemes is investigated in an analysis that goes beyond perturbation theory in the coherent driving field. In addition we examine the case where the two-photon pump field is sufficiently strong to necessitate a nonperturbative treatment. This allows us to examine the cases where either one or both of the driving fields are strong. Phase matching is included in a plane-wave propagation treatment that matches the situation most likely to be encountered in actual experiments. The calculations are in part intended to model real experimental situations and thus incorporate driving and pump-field linewidths via the phase-diffusion model and Doppler broadening. With a strong pump-field laser, large enhancements in the efficiency of light generation occur at frequencies corresponding to the Autler-Townes satellites induced by the strong driving field. In this situation gain and high four-wave-mixing efficiency are simultaneously present, resulting in the production of a large intensity of coherent radiation. \textcopyright{} 1996 The American Physical Society.
The explicit solution is obtained for Raman four-wave mixing ω4=ω1−ω2+ω3\omega_4=\omega_1-\omega_2+\omega_3ω4​=ω1​−ω2​+ω3​ of two strong fields E1,E3E_1, E_3E1​,E3​ and two weak fields E2,E4E_2, E_4E2​,E4​ in a four-level system with the large Doppler broadening. The resonance of the mixing coefficient vs intensity is found near equal Rabi frequencies of strong fields and interpreted as an intersection of quasi-energy levels. Up to 6 peaks appear in the dependence of conversion coefficient on the detuning of the probe field. An unexpected additional pair of peaks is a result of averaging over velocities and disappears at low temperature. The effects allow explaining saturation behavior in recent experiments on the mixing in sodium molecular vapor.