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Physical Review A

Effect of optical pumping and Raman scattering on the degenerate four-wave mixingin coherently pumped rubidium atoms

Yifu Zhu, T. N. Wasserlauf, Paul Sanchez

Published Jan 1, 1997• 5 citations
Publisher

Abstract

We present an experimental study of cw degenerate four-wave mixing (DFWM) in Doppler-broadened rubidium atoms coupled by an additional coherent field. The coupling field and the DFWM fields were arranged in a \ensuremath{\Lambda}-type configuration from the rubidium ${\mathrm{D}}_{2}$ transitions. We found that the presence of the coherent coupling field modifies the DFWM emission:mfat lower intensities of the coupling field, the DFWM emission is enhanced; at higher intensities of the coupling field, the DFWM is reduced. The observed effect of the coupling laser on the DFWM emission may be explained by the direct competition between the resonance-enhanced two-photon Raman scattering and the optical-pumping-enhanced DFWM emission.

DOI
10.1103/physreva.55.668

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We present an experimental study of cw degenerate four-wave mixing (DFWM) in Doppler-broadened rubidium atoms coupled by an additional coherent field. The coupling field and the DFWM fields were arranged in a \ensuremath{\Lambda}-type configuration from the rubidium D2{\mathrm{D}}_{2}D2​ transitions. We found that the presence of the coherent coupling field modifies the DFWM emission:mfat lower intensities of the coupling field, the DFWM emission is enhanced; at higher intensities of the coupling field, the DFWM is reduced. The observed effect of the coupling laser on the DFWM emission may be explained by the direct competition between the resonance-enhanced two-photon Raman scattering and the optical-pumping-enhanced DFWM emission.
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.
We present an experimental study of cw nearly degenerate four-wave-mixing emission in a Doppler broadened Rb atomic system. With the fixed detuning of an intense pump laser for the Rb D2{\mathit{D}}_{2}D2​ line, the nearly degenerate four-wave-mixing emission exhibits three peaks as a probe laser is scanned across the same Rb D2{\mathit{D}}_{2}D2​ line. The observed three-peaked spectrum can be interpreted as the resonances in the energy structure of the dressed atomic states.
The evolution of enhanced four-wave mixing based on Raman coherence as the probe intensity increases is observed experimentally in an 85 R b atomic vapor system. We propose that for a Doppler-broadened Λ -type level system, the generated anti-Stokes field from one-photon resonance will be suppressed by the dressed-states resonance and can be controlled by the probe intensity, which influences the effective transverse relaxation rate of Raman coherence. When the probe field is not so weak, the double resonance for dressed states will greatly suppress the anti-Stokes emission at the central frequency, and the signal peak will be split. We show that this phenomenon is a result of the destructive polarization interference between atoms with different velocities from the two types of resonance. Based on our model, we present a new, to the best of our knowledge, interpretation of four-wave mixing enhancement in the conventional Λ -type electromagnetically induced transparency system.
We observe experimentally huge enhanced four-wave mixing based on Raman resonance in an 85Rb atomic vapor system. With the decrease of coupling field power or the increase of experimental temperature, the signal tends to be narrowed down in linewidth, and be basically the same spectrum as the stimulated Raman spectroscopy. It is found that the macroscopic polarization interference effect plays a crucial role in determining the nonlinear spectra. Further more, in the Doppler-broadened Λ-type energy level system, there is a strong relationship among electromagnetically induced transparency, four-wave mixing and stimulated Raman spectroscopy. The sharp transparent window in electromagnetically induced transparency can be interpreted as the suppression of Raman gain on the linear absorption of the probe field. However, the four-wave mixing signal is a new field generated by the atomic vapor system, and it comes from the Raman gain which is affected and modified by the absorption and dispersion of the nonlinear optical medium. It shows that in a Λ-type Doppler-broadened system, in essence, both the electromagnetically induced transparency and enhanced four-wave mixing stem from stimulated Raman scattering based on the third-order nonlinear processes, just the spectra of which are from different ways and objects of detection.
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.
In this work, we present a set of experiments involving four-wave mixing processes in rubidium atoms. We employ several experimental configurations exploring two- and three-level systems in cascade or Λ configurations, all of which are in a copropagating geometry, to investigate different physical phenomena present in each scenario. In the first experiment, we combine a cw diode laser and a 1 GHz femtosecond pulse train to generate coherent blue light through the four-wave mixing process in hot rubidium vapor. The generated coherent signal is analyzed by scanning either the diode frequency or the repetition rate of the frequency comb. In both cases, the cw laser induces an Autler- Townes splitting with a wide separation in the doublet structure due to the configuration of copropagating fields. To model these results, we employ the density matrix formalism to write the Bloch equations and solve them numerically. The solutions allow us to explore other cases beyond those involving our experimental setup, comparing the response of the upper-level population and the generated signal coherence for homogeneously and non-homogeneously broadened systems. Moreover, in this same experiment, we also observed an unexpected interference effect between excitation routes of the four-wave mixing process when the repetition rate of the pulse train is scanned. The theoretical model demonstrates that the interfering effect appears only when the repetition rate is carefully chosen to produce a pair of modes of the frequency comb resonant with both one- and two-photon transitions for the same atomic velocity group. In the second experiment, still with a hot rubidium vapor, we explore two symmetrical degenerate four- wave mixing signals induced by two almost copropagating laser beams, with~ka and~kb wave-vectors, and detected simultaneously in the 2~ka −~kb and 2~kb −~ka directions. Each spectrum has a single peak with a short frequency separation between them, which our model indicates is due to the nonlinear behavior of the refractive indexes, a consequence of the high intensity of both input fields. Finally, we use the same experimental setup for the two symmetrical signals to study the field intensity fluctuations of the degenerate four-wave mixing signals and the transmission signals. In this case, the sample is an ensemble of cold rubidium atoms in a magneto-optical trap. There is an intensity- intensity cross-correlation between the signals due to the resonant phase-noise to amplitude-noise conversion. In this type of cold system, we can neglect the Doppler- broadening, allowing a straightforward study of the dependency of the correlations on the laser detuning. In these measurements, we observe a type of oscillation in the correlation curves that the theoretical model indicates to be connected with Rabi oscillations, revealed by the fluctuations long after the transient period.