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Physical Review A

Stochastic field-induced nonlocal resonances in four-wave mixing

Michael Scott Belsley, M. Kaczmarek, P. Ewart

Published Nov 14, 2001• 2 citations
Publisher

Abstract

We explore theoretically the signal generated by a fluctuating radiation field via a four-wave mixing process in an atomic vapor undergoing Markovian dephasing collisions. We consider specifically a broadband laser field well detuned from the atomic resonance and calculate the signal generated using counterpropagating pump fields as a function of the time delay of the incident probe field. We assume that the pulse duration is long compared to the correlation time of the incident fields. By considering the various time-ordered pathways and treating the incident-field amplitudes as random Gaussian variables, we find that the signal generated is dominated by two specific pathways that depend only on the incident-field bandwidth and the decay rate of the ground to excited state coherence. An interesting aspect of the far-impact-detuning case is that the signal is dominated by resonances involving spatially separated atoms. Our formalism provides a basis for describing the effects of mode correlations on four-wave-mixing signals generated by stochastic fields.

DOI
10.1103/physreva.64.063806

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We explore theoretically the signal generated by a fluctuating radiation field via a four-wave mixing process in an atomic vapor undergoing Markovian dephasing collisions. We consider specifically a broadband laser field well detuned from the atomic resonance and calculate the signal generated using counterpropagating pump fields as a function of the time delay of the incident probe field. We assume that the pulse duration is long compared to the correlation time of the incident fields. By considering the various time-ordered pathways and treating the incident-field amplitudes as random Gaussian variables, we find that the signal generated is dominated by two specific pathways that depend only on the incident-field bandwidth and the decay rate of the ground to excited state coherence. An interesting aspect of the far-impact-detuning case is that the signal is dominated by resonances involving spatially separated atoms. Our formalism provides a basis for describing the effects of mode correlations on four-wave-mixing signals generated by stochastic fields.
Coherent signals induced by fundamentally incoherent phenomena through a four-wave mixing process are among the most intriguing and subtle effects in nonlinear spectroscopy. These effects were initially observed by Bloembergen and his co-workers in the form of pressure-induced extra resonances in four-wave mixing. Using standard perturbance techniques based on the optical Bloch equations, they suggested that these collision induced resonances were the result of a destruction of the destructive interference existent between two alternate time-ordered pathways. Subsequently, Prior et al realised that fluctuations in the incident radiation fields could play essentially the same role as the collisionally induced dephasing. In practice, of course, both collisional dephasing and field fluctuations are present in a typical atomic vapor pulsed four-wave mixing experiment. If the timescales governing these two effects approach one another, one can expect to gain valuable new insight into this fascinating process of incoherently inducing a coherent signal
The effect of pump fluctuations on various coherent processes that arise in three-level systems interacting with two external fields is examined. Such coherent processes include the forward Hanle effect and various four-wave mixing effects such as the generation of phase-conjugate signals. A general formulation that enables one to calculate the influence of laser linewidth on the coherent signals produced in various directions is presented. Ensemble averages, over laser temporal fluctuations, of various physical quantities, such as atomic polarization, are calculated. The spectrum of polarization fluctuations is shown to consist of several new features which lead to coherent radiation in different directions depending on the resonant frequencies in the polarization fluctuations. The influence of pump linewidth on pressure-induced extra resonance (PIER) is treated in detail. The possibility of producing a laser-fluctuation-induced coherent signal at one of the atomic frequencies is examined. This new signal, which is produced in a direction different from that of the PIER signal, but has the same type of resonant character as PIER, is found to have significantly different pressure dependence than the PIER signal. The results of our numerical computations are qualitatively explained in terms of the convolutions of products of third-order susceptibilities and pump field-correlation functions.
The spectral line shape of the four-wave mixing (FWM) signal, induced by broad bandwidth laser fields, is derived in the case of a nonresonant interaction. The laser fields are assumed to have a Lorentzian spectrum arising from Markovian stochastic fluctuations described by the phase-diffusion, chaotic field, and Gaussian-amplitude models. The usual ``phase conjugating'' geometry for FWM is considered where the nonresonant interaction is determined only by the statistics of, and the correlations between, the pump and probe fields. For each one of the four possible correlation states between the three input fields and for each of the three fluctuating field models, the line shape of the FWM signal is calculated and shown to be particularly sensitive to the field statistics.
A unified approach is presented for the treatment of stochastic fluctuations in four-wave-mixing processes, including uncorrelated and fully or partially cross-correlated input laser fields. The theory allows for phase as well as amplitude fluctuations and covers Markovian and non-Markovian (non-Lorentzian) input line shapes. The analogy between laser field fluctuations and molecular dephasing processes is discussed, and several types of fluctuation-induced resonances are considered. Uncorrelated input fields give rise to resonances similar to those described previously by Agarwal, while correlated input fields cause extra resonances of the type presented by us in earlier publications. Partial cross-correlations are treated here for the first time, with predictions for new effects: Oscillations in the intensity of the generated four-wave-mixing signal as a function of the degree of cross-correlation. The conditions for the experimental observation of these effects are discussed.
We develop a theory of near-resonant four-wave mixing induced by broad-bandwidth chaotic fields in a medium composed of two-level atoms. By solving the equations of motion for the elements of the atomic density matrix using an appropriate decorrelation approximation, we derive an analytic expression for the frequency spectrum of the signal wave for the case of the bandwidth of the fluctuations of the pump field exceeding the other relaxation rates in the problem. The probe wave is considered weak and of arbitrary bandwidth. The theory is valid for pump intensities up to and exceeding the bandwidth-dependent saturation value. Finally, we show how the frequency spectrum is modified if account is taken of atomic motion. The theoretical results are of direct relevance to practical experiments involving broad-bandwidth pulsed lasers and employing an atomic vapor as the nonlinear medium.
We consider the generation of four-wave-mixing signals by an ensemble of two-level atoms interacting with broadband, correlated, pump and probe fields in the forward geometry. We show how the calculation of the four-wave-mixing signal reduces to the solution of six coupled Langevin equations that are numerically integrated using Monte Carlo methods. We account for the pump-induced saturation effects although the probe is weak. The finite correlation time of the pump and probe fields is also included. For weak and \ensuremath{\delta}-correlated pump fields, we reproduce the results of Morita and Yajima [Phys. Rev. A 30, 2525 (1984)]. We find that even for short correlation times of the fields, the four-wave-mixing signal, as a function of the delay between the pump and the probe fields, starts reviving with increase in the pump intensity. This revival as a function of the pump-probe delay time becomes more pronounced with further increase in the pump intensity.