Nonlinear optical response of three-level systems

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Abstract
We investigate the properties of a homogeneously broadened three‐level system interacting with two optical fields, Eω1(x,t) and Eω2(x,t), with central frequencies ω1 and ω2 whose amplitudes are assumed to be slowly varying in time compared with dephasing times of the optical transitions. We calculate Raman susceptibilities allowing each transition to be induced by both fields and without employing the rotating wave approximation (RWA); this enables correct calculation of the optical response of the medium when the fields are on‐resonance or arbitrarily far off‐resonance with the Raman transition. In some frequency regions the RWA causes substantial errors. A distinction is drawn between two different types of RWA: (a) a neglect of off‐resonant components of the polarization for direct optical transitions, and (b) neglect of off‐resonant components of off‐diagonal density matrix elements of order Eω1(x,t)Eω2(x,t)* in the field amplitudes. The first RWA is known to become inaccurate when the pump frequency is significantly off‐resonance with the pump transition. We show that the second RWA becomes inaccurate when ‖ω1−ω2‖ is small or comparable to the active Raman mode frequency (even when the field are close to resonance). Calculations based upon our expressions show that when the pump frequency is close to resonance with the optical transition from the ground state, a nonlinear absorption at the Stokes shifted frequency occurs. This absorption can significantly decrease the Raman gain. Also, we find that Rabi splittings in a three‐level system can occur even when the pulse durations of the incident fields are short compared with the T1 times of the system. We solve analytically for the optical response of the system to two fields of arbitrary strength and frequency. We analyze this solution and its perturbative expansion in the field amplitudes. We use the Maxwell–Bloch equations developed here to propagate time‐dependent pulses.