The exponential gain predicted in "Weak-wave advancement in nearly collinear four-wave mixing" [Opt. Express 10, 581 (2002)], disappears when all interacting sidebands are properly taken into account. The demonstration closely follows well-established literature in the formally equivalent temporal domain.
The effects of finite-bandwidth excitation are incorporated into the theoretical treatment of degenerate four-wave mixing (DFWM) spectroscopy by employing a general description of applied electromagnetic fields, thereby permitting the transient nature of typical laser sources to be taken explicitly into account. A computationally efficient perturbative (weak-field) formalism is developed by exploiting exponentially-decaying wave forms as a flexible basis for expanding the temporal envelope functions of incident quasimonochromatic pulses. This approach has the distinct advantage of yielding time-domain response integrals that can be evaluated analytically since they are almost as simple in form as their monochromatic counterparts. The resulting frequency-domain expressions for the induced DFWM signal polarization reflect the pronounced influence of finite-bandwidth excitation without needing to cobble such behavior into phenomenological rates for population decay and coherence dissipation. Spectral line shapes are examined for both stationary and nonstationary ensembles of isolated (gas-phase) target molecules, with the latter analyses demonstrating the systematic degradation of spatial discrimination introduced by nonmonochromatic implementations of the sub-Doppler (phase-conjugate) four-wave mixing scheme. In keeping with recent experimental findings, the precipitous drop in signal intensity accompanying the action of collisional dephasing processes is predicted to be tempered greatly by the use of short-duration excitation pulses.
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.