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Physical Review A

Four-wave mixing with time-delayed, correlated, phase-diffusing optical fields

Gautam Vemuri

Published Oct 1, 1993• 7 citations
Publisher

Abstract

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)].

DOI
10.1103/physreva.48.3256

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•Jan 1, 1997•0 citations
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 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.
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.
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.
Abstract : In this research program, the investigators have explored the role of fluctuations of a laser field on coherent interactions between the laser field and simple atomic systems. A key feature of these experiments is their ability to provide measurements of complex nonlinear optical interactions which are sufficient for direct, quantitative comparison with theory. The main thrust of the present work has been the study of non-Markovian field statistics, present in experiments that use multiple, time-delayed input beams to drive the nonlinear system. The specific interaction studied was Phase-Conjugate Four-Wave Mixing in an optically-pumped beam of atomic sodium, which the researchers measured as a function of laser bandwidth, Rabi frequency, and delay time between the pump and probe beams. The investigators have also calculated the expected signal strength through numerical integration of the Optical Bloch Equations. Experimental and numerical results are in very good agreement. The investigators also studied theoretically two-photon absorption with correlated, time-delayed input fields, and provided the first experimental confirmation of the fundamental theory of Phase-Conjugate Four-Wave Mixing with monochromatic fields in a simple atomic system.
We report measurements of the effect of laser fluctuations on a strong-field degenerate four-wave mixing interaction, carried out in a nearly Doppler-free, two-level system using a single laser with statistically well-defined phase fluctuations. The counterpropagating pump beams and the probe beam, each split from this phase-noise-modulated source, were fully correlated. The nonlinear medium was an optically-pumped diffuse beam of atomic sodium. By time-delaying the probe with respect to the pump beams, the composite field becomes non-Markovian. Four-wave mixing results in the generation of a phase-conjugate beam anti-parallel to the probe beam. With the laser field spectrum nearly Lorentzian in shape, and with a field linewidth greater (and, for comparison, much narrower) than the natural linewidth of the sodium, we measured the intensity of the phase-conjugate beam as the pump and probe beams were tuned through the D2 resonance, as a function of intensity of die pump beam (up to intensities several times the saturation intensity), and for varying delay between the pump and probe fields. This experiment provides a cleaner measurement of this interaction than any previously available.
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.