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Optics Letters

Coherent anti-Stokes Raman scattering in a microcavity

David Gachet, Franck Billard, Hervé Rigneault

Published Jun 2, 2009• 3 citations
Publisher

Abstract

We study tight focus coherent anti-Stokes Raman scattering (CARS) emission in a microcavity where the active medium is squeezed between two independent planar mirrors. We show strong modifications in the CARS forward and backward far-field radiation patterns. For low-order cavities, we demonstrate that most of the emitted power can be concentrated into a direction perpendicular to the mirrors.

DOI
10.1364/ol.34.001789

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We study tight focus coherent anti-Stokes Raman scattering (CARS) emission in a microcavity where the active medium is squeezed between two independent planar mirrors. We show strong modifications in the CARS forward and backward far-field radiation patterns. For low-order cavities, we demonstrate that most of the emitted power can be concentrated into a direction perpendicular to the mirrors.
The non-classical effects of squeezing of light in coherent anti-Stokes Raman scattering (CARS) and coherent anti-Stokes hyper-Raman scattering (CAHRS) are investigated under the short-time approximation based on a fully quantum mechanical approach. In an idealized model CARS, the interaction is looked upon as a process involving absorption of a pump photon and emission of a Stokes photon, which is followed by absorption of a pump photon and subsequently emission of an anti-Stokes photon at a different frequency, whereas CAHRS is looked upon as a process involving absorption of two pump photons and emission of a Stokes photon, which is followed by absorption of two more pump photons and subsequent emission of an anti-Stokes photon at a different frequency. The coupled Heisenberg equations of motion involving real and imaginary parts of the quadrature operators are established. It is shown that squeezing in the Stokes and anti-Stokes mode in CARS is found to be dependent on amplitude-squared squeezing of the initial pump field while, in CAHRS, it is dependent on the fourth-order amplitude squeezing of the initial pump field. Higher-order squeezing can be converted to linear squeezing through these processes. It is also shown that squeezing is greater in CAHRS than the corresponding squeezing in CARS.
Coherent anti-Stokes Raman scattering (CARS) interferometry is used to deplete the anti-Stokes radiation emerging from a tightly focused spot. Near-to-complete depletion of the anti-Stokes radiation is obtained when a phase-controlled local oscillator field at the anti-Stokes frequency is out of phase with the induced CARS field in the focal volume. Unlike in traditional interferometry, this depleted energy is not spatially redistributed. A theoretical analysis shows that the energy loss in the anti-Stokes channel is accompanied by an energy gain in the pump and Stokes channels. Interferometric switching of anti-Stokes radiation may offer a route toward developing high-resolution CARS microscopy.
We report the measurement of degenerate coherent anti-Stokes Raman scattering (CARS) in a high-finesse optical microcavity, with an atmospheric gas as the nonlinear medium. Unlike the well-known bulk process in which index-dispersion compensation is required for phase-matching, efficient microcavity CARS involves a resonant coupling at the Stokes, pump, and anti-Stokes frequencies which can be described using coupled-mode analysis. We show how the interaction is thereby dramatically enhanced in a microscopic sample volume and illustrate the technique for the measurement of CO₂ in air.
The optical response used in studies of coherent anti-Stokes Raman scattering (CARS) microscopy can be enhanced or suppressed by means of electromagnetic confinement. In this paper, an approach based on planar mirrors is presented. Because of the classical origin of such a nonlinear optical effect, the theory is developed within a fully classical framework and it turns out that the CARS signal can be modified in a fashion similar to what has been extensively investigated for equivalent alterations of incoherent signals understood in terms of cavity quantum electrodynamics.
We theoretically investigate a scheme in which backward coherent anti-Stokes Raman scattering (CARS) is significantly enhanced by using slow light. Specifically, we reduce the group velocity of the Stokes excitation pulse by introducing a coupling laser that causes electromagnetically induced transparency (EIT). When the Stokes pulse has a spatial length shorter than the CARS wavelength, the backward CARS emission is significantly enhanced. We also investigated the possibility of applying this scheme as a CARS lidar with O2 or N2 as the EIT medium. We found that if nanosecond laser with large pulse energy (>1 J) and a telescope with large aperture (~10 m) are equipped in the lidar system, a CARS lidar could become much more sensitive than a spontaneous Raman lidar.