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Journal of the Optical Society of America B

Competition between four-wave mixing and incoherent nonlinear optical processes

Michelle S. Malcuit, Daniel J. Gauthier, Robert W. Boyd

Published Jan 1, 1986• 0 citations
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Abstract

When a strong near-resonant laser beam propagates through an atomic vapor, it can simultaneously induce several different nonlinear optical processes. In certain restricted conditions, these processes evolve independently of one another, but in general these processes compete. We have observed competition1 between four-wave mixing2 (FWM) and amplified spontaneous emission3 (ASE) and have presented an explanation for this phenomenon based on the solution of the coupled-amplitude equations of nonlinear optics. We extend our previous work by presenting a more detailed theoretical explanation of this effect and evidence that competition of this sort occurs quite generally in nonlinear optical systems.

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Competition between amplified spontaneous emission and the four-wave-mixing process

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Competition between amplified spontaneous emission (ASE) and the four-wave-mixing (FWM) process has been observed under conditions of two-photon resonant excitation of the sodium 3d level. The nature of the competition is that the FWM process is able to prevent the occurrence of ASE, even though the gain of the ASE process calculated in the absence of competition effects is much larger than that of FWM. The ASE is suppressed because the fields generated by the FWM process create a new excitation pathway connecting the ground and 3d levels, and under quite general conditions this pathway interferes destructively with that due solely to the applied laser field. These effects are modeled theoretically by solving perturbatively the density-matrix equations of the atomic system, thereby determining the population in the upper level and the nonlinear polarization of the medium. The coupling between the various optical fields due to the nonlinear polarization is described by coupled amplitude equations. The solution to these equations predicts that when the wave-vector mismatch is not too large the fields evolve spatially to reach steady-state values, and that the population excited to the 3d level by the total steady-state optical field is much smaller than that due to the incident laser field alone. We have observed experimentally the suppression of ASE by FWM and have observed that this suppression does not occur when the medium is excited with counterpropagating beams that cannot efficiently excite the FWM process. In addition, we have conducted a series of experiments that shows that the degree of suppression of ASE depends on the intensity and focusing characteristics of the incident laser as expected on the basis of our theoretical model.

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Competition has been observed between amplified spontaneous emission (ASE) and four-wave mixing (FWM). Previously, competition between an incoherent and coherent process was observed in the form of suppression of multiphoton ionization by third harmonic generation.1,2 In our experiment, an input laser was tuned precisely to the 3s → 3d two-photon allowed transition in atomic sodium vapor and the emission was observed in both the forward and backward directions. In these conditions, either FWM or ASE can occur. Ignoring the possibility of competition between these two processes, the calculated gain for ASE is much larger than that for FWM. However, we have observed experimentally that FWM and not ASE occur. To determine that it is the presence of efficient FWM that suppresses ASE, we have excited the atomic vapor instead with counterpropagating pump waves of different frequency. In this case, FWM, being a phase-matched process, cannot occur and strong ASE is observed. The nature of this competition is explained by solving the coupled Maxwell and density matrix equations for a three-level system. It is found that the suppression is due to the destructive interference between two different pathways of excitation of the 3d level which results in trapping of the population in the ground state.

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Instabilities in the Propagation of Laser Beams Through Atomic Vapors

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Applied Physics Letters•Aug 6, 2007•36 citations
When a strong near-resonant laser beam propagates through an atomic vapor, it can simultaneously induce several different nonlinear optical processes. In certain restricted conditions, these processes evolve independently of one another, but in general these processes compete. We have observed competition1 between four-wave mixing2 (FWM) and amplified spontaneous emission3 (ASE) and have presented an explanation for this phenomenon based on the solution of the coupled-amplitude equations of nonlinear optics. We extend our previous work by presenting a more detailed theoretical explanation of this effect and evidence that competition of this sort occurs quite generally in nonlinear optical systems.
Competition between amplified spontaneous emission (ASE) and the four-wave-mixing (FWM) process has been observed under conditions of two-photon resonant excitation of the sodium 3d level. The nature of the competition is that the FWM process is able to prevent the occurrence of ASE, even though the gain of the ASE process calculated in the absence of competition effects is much larger than that of FWM. The ASE is suppressed because the fields generated by the FWM process create a new excitation pathway connecting the ground and 3d levels, and under quite general conditions this pathway interferes destructively with that due solely to the applied laser field. These effects are modeled theoretically by solving perturbatively the density-matrix equations of the atomic system, thereby determining the population in the upper level and the nonlinear polarization of the medium. The coupling between the various optical fields due to the nonlinear polarization is described by coupled amplitude equations. The solution to these equations predicts that when the wave-vector mismatch is not too large the fields evolve spatially to reach steady-state values, and that the population excited to the 3d level by the total steady-state optical field is much smaller than that due to the incident laser field alone. We have observed experimentally the suppression of ASE by FWM and have observed that this suppression does not occur when the medium is excited with counterpropagating beams that cannot efficiently excite the FWM process. In addition, we have conducted a series of experiments that shows that the degree of suppression of ASE depends on the intensity and focusing characteristics of the incident laser as expected on the basis of our theoretical model.
Competition has been observed between amplified spontaneous emission (ASE) and four-wave mixing (FWM). Previously, competition between an incoherent and coherent process was observed in the form of suppression of multiphoton ionization by third harmonic generation.1,2 In our experiment, an input laser was tuned precisely to the 3s → 3d two-photon allowed transition in atomic sodium vapor and the emission was observed in both the forward and backward directions. In these conditions, either FWM or ASE can occur. Ignoring the possibility of competition between these two processes, the calculated gain for ASE is much larger than that for FWM. However, we have observed experimentally that FWM and not ASE occur. To determine that it is the presence of efficient FWM that suppresses ASE, we have excited the atomic vapor instead with counterpropagating pump waves of different frequency. In this case, FWM, being a phase-matched process, cannot occur and strong ASE is observed. The nature of this competition is explained by solving the coupled Maxwell and density matrix equations for a three-level system. It is found that the suppression is due to the destructive interference between two different pathways of excitation of the 3d level which results in trapping of the population in the ground state.
Two four-wave mixing (FWM) processes with different directions and frequencies can coexist and interfere in a four-level inverted-Y-type atomic system, the generated FWM beams fall into two different electromagnetically induced transparency windows. We report Autler-Townes splitting and dressed suppression and enhancement of two generated FWM beams. In the case of matched slow FWM beams, two FWM processes compete and exchange their energies between them, the forward four-wave beam give its energy to the backward four-wave beam by interaction for long distance. Such studies of two FWM beams can have vital applications in studying the higher-order nonlinear optical processes, generating correlated photon pairs and quantum information processing.
There are several nonlinear optical processes that can lead to instabilities in a laser beam as it propagates through a nonlinear optical medium. Self focusing effects, for instance, can lead to the growth of new spatial frequency components in a laser beam. A laser beam can also be unstable to the growth of new spectral components. Stimulated Raman scattering is a well-known example of a process that can lead to this sort of instability. In this paper, we present the results of a series of experiments on the somewhat different instabilities that occur for the case of the propagation of a laser beam through an atomic vapor. We find that these instabilities become particularly pronounced when the frequency of the incident laser is near to that of a one- or two-photon resonance of the atom. In either case, we find that the laser beam is unstable to the growth of new frequency components, and that in general these new frequencies are not emitted collinearly with the incident laser. These instabilities are important because they place a limit on the laser intensity that can be used to drive nonlinear optical processes.
We experimentally investigate the soliton formation and dynamics in the nonlinear propagation of the generated signal and probe beams in four-wave mixing (FWM) process with atomic coherence in a three-level atomic system, under the competition between focusing and defocusing nonlinearities, as well as between gain and dissipation, due to the third- and fifth-order nonlinear susceptibilities with opposite signs. With multi-parameter controllability and nonlinear competition in the system, fundamental, dipole, and azimuthally-modulated vortex FWM solitons can transform mutually from one to the other. Such investigations have potential applications in optical pattern formation and control, and all-optical communication.
Two four-wave-mixing (FWM) processes can coexist in a four-level Y-type atomic system with carefully arranged coupling laser beams. The generated two FWM signal beams fall into two simultaneously opened dual electromagnetically induced transparency (EIT) windows, which can be tuned to overlap or separate by various frequency detunings. The authors report our experimental observation of competing FWM processes, especially mutual suppression of the two FWM signals when the two EIT windows merge in frequency. Controlling FWM processes can have important applications in wavelength conversion for optical communication.