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arXiv:1901.00459

Coherent Anti-Stokes Raman scattering in optically active medium

Tuguldur Begzjav, Marlan O. Scully, G. S. Agarwal

Published Jan 2, 2019• 0 citations
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Abstract

Early theoretical works on coherent anti-Stokes Raman scattering in optically active medium consider only heterodyne signal and subsequently, fourth- and fifth-rank tensor averages have been used. In this work, we presented a full signal expression of coherent anti-Stokes Raman scattering in optically active medium with the help of eighth- and ninth-rank tensor averaging for simplest experimental configuration namely, measurements of post-selected circularly polarized components of scattered anti-Stokes field in the presence of three incident laser beams all linearly polarized along the same axis.

DOI
10.48550/arxiv.1901.00459

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Early theoretical works on coherent anti-Stokes Raman scattering in optically active medium consider only heterodyne signal and subsequently, fourth- and fifth-rank tensor averages have been used. In this work, we presented a full signal expression of coherent anti-Stokes Raman scattering in optically active medium with the help of eighth- and ninth-rank tensor averaging for simplest experimental configuration namely, measurements of post-selected circularly polarized components of scattered anti-Stokes field in the presence of three incident laser beams all linearly polarized along the same axis.
The optical mixing of sufficiently coherent radiations of frequency (omega) 1 and (omega) 2 inside a suitable molecular medium can result coherent radiation at new frequency (omega) 3 equals [(omega) 1 + ((omega) 1 - (omega) 2)]. If (omega) 1 is kept fixed and (omega) 2 is varied so that a condition (omega) 1 - (omega) 2 equals (omega) is reached where (omega) is a molecular frequency of the medium, then (omega) 3 equals (omega) 1 + (omega) equals 2(omega) 1 - (omega) 2. In this case (omega) 3 coincides with the anti- Stokes Raman frequency associated with the molecular frequency (omega) . This process of coherent anti-Stokes Raman Scattering (CARS) is an important nonlinear optical process which provides intense collimated signal beams and is also an excellent spectroscopic tool. CARS being a four-wave mixing process, it is of interest to study the process in multi-level system to obtain a better insight into the problem. In the current paper we investigate the different quantum statistical properties of CARS in a inhomogeneously broadened three-level system based on density-matrix formalism where both the atomic system and the radiation fields are quantised. The photon-statistics, coherence characteristics and the occurrence of anti-bunching of the CARS field, in the steady state, are investigated.
Spatial symmetries inherent to tight focus optical beams are applied to control the field phase generated at interfaces in nonlinear optical processes. We use these symmetries to obtain a background-free pure Raman spectrum in coherent anti-Stokes Raman scattering spectroscopy from a resonant medium forming a transverse interface with a nonresonant medium. We demonstrate that the nonresonant medium acts as a local oscillator with which the Raman spectrum is measured in heterodyne detection. This method is relevant to remove the nonresonant background in other third-order resonant processes excited with focused beams.
Raman oscillation, frequency upconversion, and Raman amplification can be achieved in a second-order nonlinear medium at the phonon-polariton resonance. By beating two optical fields, a second-order nonlinear polarization is generated inside the medium. Such a polarization induces a spatially uniform nonpropagating electric field at the beat frequency, which in turn mixes with the input optical field at the lower frequency to generate or amplify the anti-Stokes optical field. Raman oscillation can be efficiently reached for the copropagating configuration. In comparison, efficient frequency upconversion and large amplifications are achievable for the counterpropagating configuration. These Raman processes can be used to effectively remove transverse-optical phonons before decaying to lower-frequency phonons, achieve laser cooling, and significantly enhance coherent anti-Stokes Raman scattering. The counterpropagating configuration offers advantages for amplifying extremely weak signals.
Coherent Raman scattering can generate Stokes and anti-Stokes fields of comparable intensities. When the Raman shift is due to a magnetic resonance transition (usually in the MHz to GHz range), the Raman fields are generally detected by optical heterodyne detection, using the excitation laser as the local oscillator. In this case, the two sidebands generate beat signals at the same frequency and are therefore indistinguishable. Separation of the two contributions becomes possible, however, by superheterodyne detection with a frequency-shifted optical local oscillator. We compare the two scattering processes, and show how the symmetry between them can be broken in Pr3+:YAlO3.{\mathrm{Pr}}^{3+}{:\mathrm{Y}\mathrm{A}\mathrm{l}\mathrm{O}}_{3}.Pr3+:YAlO3​.
In the coherent anti-Stokes Raman scattering process, the spectrum of the generated optical phonon depends on the degree of temporal correlation between the pump laser field and the Stokes field. When the two fields are strongly correlated, such as when the Stokes field is generated with stimulated Raman scattering (SRS), the spectral shape of the optical phonon is found experimentally and theoretically to be the same as the gain-narrowed Raman line shape because the laser phase fluctuations cancel out totally, leaving only the collisional noise in the SRS process. When the two fields are uncorrelated, the shape of the optical-phonon spectrum is found to be the same as the Raman line shape without gain narrowing. When two fields are partially correlated, then the two spectral components appear together. We provide a method to measure the degree of correlation between two optical fields that have different central frequencies. The theory developed to interpret the experimental results is an extension of the quantum theory of SRS to include anti-Stokes scattering. We show that only in the high-gain limit can the quantum fluctuations be thought of as arising from a classical noise process.