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Optics Letters

Investigation of anti-Stokes Raman processes at phonon-polariton resonance: from Raman oscillation, frequency upconversion to Raman amplification

Yujie J. Ding

Published Feb 18, 2015• 4 citations

Abstract

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.

DOI: 10.1364/ol.40.000729

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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

{\mathrm{Pr}}^{3+}{:\mathrm{Y}\mathrm{A}\mathrm{l}\mathrm{O}}_{3}.

The anti-Stokes Raman laser process is an interesting method for frequency upconversion and generation of tunable UV radiation. This method requires no index matching and allows high-conversion efficiencies and output energies and large frequency shifts in a single step. A basic requirement is a population inversion between a metastable level and a suitable lower-lying level. So far anti- Stokes laser emission has been demonstrated using the metastable TI (6P3/2). l(5P1/2). and Br (4P1/2) levels, where a population inversion with respect to the corresponding atomic ground states has been generated by photodissociation of suitable compounds.1-3 For the Tl system efficiencies of 10 % and output energies of ~1 mJ (at 377 nm) have been reported,1 and with Br a shortest wavelength of 149 nm was possible by upconversion of 157.5-nm radiation of a F2 laser.3

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.

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.