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Physical Review A

Comparative study of four-wave mixing in chaotic and phase-diffusing fields

G. S. Agarwal, Gautam Vemuri, C. V. Kunasz, J. Cooper

Published Nov 1, 1992• 11 citations
Publisher

Abstract

We consider the dependence of the four-wave-mixing signal from an ensemble of homogeneously broadened, two-level atoms on the statistics of the pump field. Two models for the pump field are considered: the chaotic field and the phase-diffusing field. A Monte Carlo simulation procedure is used to integrate the equations describing the four-wave-mixing process numerically. This technique allows consideration of arbitrary bandwidths for the pump and incorporates pump-induced saturation effects. Results are presented for the strength of the four-wave-mixing signal as a function of the pump intensity for both resonant and off-resonant cases. It is shown that the four-wave-mixing signal is sensitive to the statistics of the pump, particularly for strong fields.

DOI
10.1103/physreva.46.5879

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•Jan 1, 1997•0 citations
We consider the dependence of the four-wave-mixing signal from an ensemble of homogeneously broadened, two-level atoms on the statistics of the pump field. Two models for the pump field are considered: the chaotic field and the phase-diffusing field. A Monte Carlo simulation procedure is used to integrate the equations describing the four-wave-mixing process numerically. This technique allows consideration of arbitrary bandwidths for the pump and incorporates pump-induced saturation effects. Results are presented for the strength of the four-wave-mixing signal as a function of the pump intensity for both resonant and off-resonant cases. It is shown that the four-wave-mixing signal is sensitive to the statistics of the pump, particularly for strong fields.
Four-wave mixing in homogeneously broadened, two-level atoms, driven by time-delayed, correlated phase-diffusing optical fields is investigated. The spectrum of the driving field has an arbitrary bandwidth, i.e., it can have a Lorentzian or a Gaussian profile or an intermediate profile (Voigt). A time delay between the strong pump and weak probe field provides a partial correlation between the fields, and this time delay makes the composite field seen by the atoms non-Markovian. It is shown that the calculation of the four-wave-mixing signal reduces to the solution of six coupled Langevin equations with multiplicative noise; Monte Carlo techniques are utilized to study the response of the atoms to non-Markovian fields. A technique for numerically simulating phase-diffusing fields with colored frequency fluctuations is shown. The four-wave-mixing profiles are found to be significantly different from those for which the driving field is chaotic. The profiles show oscillatory behavior as evidence of the Rabi frequency, a feature not seen in previous works. For some parameter values, a revival of the signal is seen for an increasing time delay, analogous to the revivals seen in chaotic field signals [Phys. Rev. A 44, 6009 (1991)].
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.
The effects of finite laser bandwidth on resonant degenerate four-wave mixing (DFWM) are calculated with use of a model in which the intense, counterpropagating pump beams are characterized by a chaotic field, the probe beam is weak and monochromatic, and the medium consists of a gas of two-level atoms. We present a steady-state solution in the limit where the pump-laser bandwidth exceeds all other atomic relaxation rates. Although the mean intensity due to the fluctuating fields is spatially independent (no steady-state standing-wave pattern is established), the analytic results indicate that, for intensities above the saturation intensity Isat{I}_{\mathrm{sat}}Isat​, spatially periodic saturation effects are important. Increasing bandwidth is shown to lead to an increase in the effective saturation intensity resulting in lower phase-conjugate reflectivity for IIsat{I}_{\mathrm{sat}}Isat​ than for coherent pump fields, in contrast to the results for narrow-bandwidth chaotic fields. The resonant DFWM line shape is also calculated and compared to the coherent result. We comment on the application of the model to other four-wave-mixing processes employing broad-bandwidth lasers.
We present results of our experimental investigations of phase-conjugate four-wave mixing in a nearly Doppler-free, collisionless, two-level quantum system with a partially coherent non-Markovian laser field. The two components of the laser field---an intense pump and a weak, time-delayed probe---are derived from a single narrow-band cw laser source on which phase and frequency fluctuations conforming to the phase diffusion model are superimposed. We carry out these measurements using the D2{D}_{2}D2​ transition in an optically pumped diffuse beam of atomic sodium. We vary the pump intensity, laser bandwidth, and temporal delay between the pump and probe, and measure the peak signal strength, the bandwidth, and the asymmetry of the four-wave-mixing spectrum. For comparison with our experimental results of the peak signal strength, we also analyze the same interaction numerically, through direct integration of the optical Bloch equations. The numerical results are in good agreement with the measurements.
In this study, we extended the observation of the effect of the coherence of a laser field to four-wave mixing interactions in atomic media. These measurements will help us understand quantitatively recent techniques employing broad-band nanosecond laser pulses for measurements of sub-picosecond dipole relaxation lifetimes in a variety of media. The coherence of the laser field in this work is controlled using random phase/frequency modulation techniques, creating a field in the laboratory known as the phase diffusion field. The four-wave mixing signal is generated by an ensemble of two-level atoms (Na) interacting with degenerate broad-band, correlated, pump and probe fields. This two-level system is produced by optically pumping the sodium atoms into a single hyperfine component of the ground state. Data sets were taken without and with noise applied to the optical field. For the latter, we measured the dependence of the power of the four-wave mixing signal on the delay times between the pump and probe beams. These data sets were compared with the computer simulation results.