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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Nonlinear interference of optical transitions under multiphoton resonances

Eduard A. Manykin

Published May 10, 1996• 0 citations
Publisher

Abstract

Phenomenon of nonlinear interference as a result of no less than two monochromatic light wave with far difference of optical frequencies is discussed by means of the function of correlation for the electrical field amplitude. The extension of the nonlinear interference theory on nonmonochromatic light waves for multiphoton resonances is represented.

DOI
10.1117/12.239494

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Phenomenon of nonlinear interference as a result of no less than two monochromatic light wave with far difference of optical frequencies is discussed by means of the function of correlation for the electrical field amplitude. The extension of the nonlinear interference theory on nonmonochromatic light waves for multiphoton resonances is represented.
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Some typical resonance nonlinear-optics phenomena taking place when light interacts with atoms are considered. The multitude of such phenomena reduces to scattering of the perturbing light, perturbation of the atomic spectrum, excitation of an atom and its ionization. In all these cases the investigations are carried out using the simplest model—an isolated atom in a monochromatic external field. Such a model enables one to give an exact description of many elementary processes. On the other hand it is sufficiently realistic. A detailed investigation is carried out of resonance fluorescence, spontaneous Raman scattering, multiphoton excitation of atoms, resonance shifts and splitting of atomic levels and resonance lonication of atoms. The nature of these processes is investigated as a function of the intensity of the external field, its frequency, a specific atomic spectrum, the nature of polarization of the perturbing field, and the degree of its nonlinearity. The role played by the field of the electromagnetic vacuum is analyzed. Theoretical predictions are compared with the results of many experiments describing resonance processes of the interaction of an intense light field with atoms.
Resonance fluorescence arises from the coherent interaction of laser light with a two-level system and constitutes a quantum light source exhibiting single-photon emission and antibunching, making it a fundamental building block for future quantum networks. Our recent work [Nat. Commun.16, 6453 (2025)10.1038/s41467-025-61884-x] demonstrates that under continuous-wave excitation and in the absence of pure dephasing, the single-time joint state of resonance fluorescence and the two-level system can be described by a pure entangled state. Here, we analyze the cross-correlation and auto-correlation properties of the quantum optical field generated by the interference of resonance fluorescence with laser light at the resonance excitation frequency. Simulation results indicate that by varying the intensity or phase of the interfering laser light, the higher-order coherence of the post-interference quantum optical field transitions from anti-bunching to super-bunching behavior, consistent with recent theoretical and experimental advances by mean-field engineering. This approach offers a complementary framework to characterize and manipulate the multiphoton quantum optical fields.
When an atom is irradiated by two light beams whose sum frequency corresponds to an allowed two-photon transition between two 1S^{1}\mathrm{S}1S states, no radiation is absorbed if the electric vectors of the two beams are perpendicular to each other. Application of a magnetic field in a direction perpendicular to the plane defined by the two electric vectors permits two-photon absorption to take place. According to quantum theory the effect is interpreted as an interference phenomenon. That is, if no field is applied, the intermediate states are degenerate and the interference is destructive; when a magnetic field is applied, two different paths through intermediate states are possible, permitting population of the upper state. The effect is related to the Hanle effect and likewise provides the basis for an experimental method of determining Land\'e factors.
We present a theory for two- and three-photon excitation, optical shifting, and four-wave mixing when a first laser is tuned onto, or near, a two-photon resonance and a second much more intense laser is tuned near or on resonance between the two-photon resonance and a second excited state. When the second excited state has a dipole-allowed transition back to the ground state and the concentration is sufficiently high, a destructive interference is produced between three-photon coupling of the ground state and the second excited state and one-photon coupling between the same states by the internally generated four-wave mixing field. This interference leads to several striking effects. For instance, as the onset of the interference occurs, the optical shifts in the two-photon resonance excitation line shape become smaller in copropagating geometry so that the line shapes for multiphoton ionization enhanced by the two-photon resonance eventually become unaffected by the second laser. In the same range of concentrations the four-wave mixing field evolves to a concentration-independent intensity. With counterpropagating laser beams the line shape exhibits normal optical shifts like those observed for both copropagating and counterpropagating laser beams at very low concentrations. The theoretical work presented here extends our earlier works by including the effect of laser bandwidth and by removing the restriction of having the second laser be tuned far from three-photon resonance. In this way we have now included, as a special case, the effect of both laser bandwidth and interference on laser-induced transparency. Unlike other effects related to odd-photon destructive interference, the effect of a broad bandwidth is to bring about the predicted effects at much lower concentrations. Studies in rubidium show good agreement between theory and experiment for both ionization line shapes and four-wave mixing intensity as a function of concentration.