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Physical Review A

Phase-conjugate four-wave mixing with partially coherent laser fields

Binh Do, Jongwhan Cha, Daniel S. Elliott, Stuart James Smith

Published Jul 1, 1999• 5 citations
Publisher

Abstract

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 ${D}_{2}$ 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.

DOI
10.1103/physreva.60.508

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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 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.
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 present experimental observations of phase-conjugate degenerate four-wave mixing in a two-level atomic system (the ${3s}^{2}{S}_{1/2}, F=2, {m}_{F}=\stackrel{\ensuremath{\rightarrow}}{2}{3p}^{2}{P}_{3/2}, F=3, {m}_{F}=3$ transition in a diffuse, collision-free, thermal beam of atomic sodium) driven by cw, narrow-band $(\ensuremath{\sim}250 \mathrm{kHz}),$ stabilized pump and probe fields. The primary measurements that we report are of the peak signal strength of the four-wave-mixing interaction and the bandwidth of the four-wave-mixing spectrum (as the laser frequency is tuned through the resonant frequency) as a function of the intensity of the pump field. We compare these measurements with the predictions of a theoretical analysis in which extension to include the effect of the small transverse velocity $(\ensuremath{\sim}3 \mathrm{m}/\mathrm{s}\mathrm{e}\mathrm{c})$ of the atomic beam is critical. These measurements provide a direct verification of the theory of this important nonlinear interaction.
We study phase-conjugate degenerate four-wave mixing (DFWM) in an optically pumped, two-level atomic system (the 3s2S1∕23s\phantom{\rule{0.2em}{0ex}}^{2}S_{1∕2}3s2S1∕2​, F=2F=2F=2, ${m}_{F}=2\ensuremath{\rightarrow}3p\phantom{\rule{0.2em}{0ex}}^{2}P_{3∕2}$, F=3F=3F=3, mF=3{m}_{F}=3mF​=3 transition in a diffuse, collision-free, thermal beam of sodium) using phase-modulated laser beams. In this investigation, we study the detailed line shape of the four-wave mixing signal as a function of the temporal delay between the probe field and the pump fields at different intensities of the cw pump waves and modulation frequencies. We show that phase modulation of the pump and probe beams leads to strong amplitude modulation of the phase-conjugate beam and report excellent agreement between our experimental observations of the DFWM spectra and the results of numerical calculations. Our numerical results suggest an enhancement of the ``local'' DFWM signal when the sidebands of the phase-modulated laser are resonant with dressed-state transitions, but that this resonance is less obvious in the total signal generated. We also show that the complex line shapes depend sensitively upon the delay of the probe beam, with the peak DFWM signal occurring when the probe beam is advanced compared to the pump beam.
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.
We study phase-conjugate degenerate four-wave mixing in an optically pumped, two-level atomic system (the 3s2S1/2,{3s}^{2}{S}_{1/2},3s2S1/2​, F=2,F=2,F=2, ${m}_{\mathrm{F}}=\stackrel{\ensuremath{\rightarrow}}{2}{3p}^{2}{P}_{3/2},$ F=3,F=3,F=3, mF=3{m}_{\mathrm{F}}=3mF​=3 transition in a diffuse, collision-free, thermal beam of sodium). In this investigation, we study the detailed line shape and strength of the four-wave mixing signal as a function of the intensity of the cw pump waves, and of the velocity of the atoms. Our technique allows us to examine the four-wave mixing interaction under conditions in which the Doppler shift, the natural linewidth of the transition, and the Rabi frequency for the interaction are each comparable with one another. From our experimental measurements and computational results, we show that the line shapes are very complex in this regime, and that they depend sensitively upon the atomic velocity, especially in the case when the intensity of the forward and backward pump beams exceeds the saturation intensity for the transition.