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Journal of the Optical Society of America B

Interference between competing quantum-mechanical pathways for four-wave mixing

Philip B. Chapple, K. G. H. Baldwin, Hans‐A. Bachor

Published Feb 1, 1989• 13 citations
Publisher

Abstract

The interference between two different quantum-mechanical pathways for four-wave mixing in sodium vapor has been observed. The four-wave mixing was enhanced by two-photon resonance with the 5s state, for one pathway, and the 4d state, for the other. The phase of the interference could be varied continuously by varying laser frequencies, and constructive and destructive interference effects were studied. A model based on third-order perturbation theory gives a good description of the features observed.

DOI
10.1364/josab.6.000180

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The interference between two different quantum-mechanical pathways for four-wave mixing in sodium vapor has been observed. The four-wave mixing was enhanced by two-photon resonance with the 5s state, for one pathway, and the 4d state, for the other. The phase of the interference could be varied continuously by varying laser frequencies, and constructive and destructive interference effects were studied. A model based on third-order perturbation theory gives a good description of the features observed.
Two-photon-resonant excitation of the sodium 3d3d3d level can lead to the generation of new frequencies either by amplified spontaneous emission at the $3d\ensuremath{\rightarrow}3p$ transition frequency or by a resonantly enhanced four-wave mixing process. Competition between these two processes has been observed. The four-wave mixing process can suppress amplified spontaneous emission by preventing the excitation of the 3d3d3d level due to an interference between two different pathways connecting the ground (3s3s3s) and 3d3d3d states.
In femtosecond degenerate four-wave mixing experiments in sodium vapor, quantum beats are observed at the wavelength of the third harmonic when the fundamental beams are three-photon resonant. The period of beating, which corresponds to fine structure energy-level splitting, does not change with the atomic number density, buffer gas pressure, or laser intensity. Surprisingly, the third-harmonic signal is observed only at negative time delays for the transient grating pulse sequence. We relate this to the well-known interference effect between excitation pathways involving the fundamental and the third-harmonic fields, which leaves atoms virtually unexcited and prevents formation of population grating.
We have observed an interference in four-wave mixing involving two Rydberg states that play the key role of near two-photon resonant intermediate levels. This interference, due to the coherence of the nonlinear process, can be explained either classically or quantum mechanically and it depends on the lasers' polarizations and detunings. We have performed calculations that are in very good agreement with the experimental data. Our results provide new information about the system, such as ionization rates of the Rydberg levels and the ratio of reduced matrix elements involved.