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Optical Engineering

Abnormal anti-Stokes Raman scattering and coherent backscattering as manifestation of Anderson localization of light in nonlinear mesoscopic materials

Ion Smaranda, Lucian Mihut, Mihaela A. Baibarac, Ioan Baltog, S. Lefrant

Published Sep 19, 2014• 2 citations
Publisher

Abstract

We demonstrate that under continuous single-beam excitation, one can generate an abnormal anti-Stokes Raman emission (AASRE) whose properties are similar to a coherent anti-Stokes Raman scattering. The effect has been observed in mesoscopic materials, which possess intrinsically nonlinear properties [lithium niobate (LiNbO3), bismuth germanium oxide (Bi12GeO20; BGO), bismuth silicon oxide (Bi12GeO20; BSO)], which have a nonzero electric susceptibility of the third order, χ(3)≠0. Corroborated Raman and coherent backscattering studies demonstrate that the occurrence of both effects is conditioned by the existence of a mesoscopic morphology of the sample, which is able to ensure efficient transport of the light inside the sample through a multiple light scattering mechanism. In this context, both AASRE and coherent backscattering effects are because of the Anderson localization of the light.

DOI
10.1117/1.oe.53.9.097109

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We demonstrate that under continuous single-beam excitation, one can generate an abnormal anti-Stokes Raman emission (AASRE) whose properties are similar to a coherent anti-Stokes Raman scattering. The effect has been observed in mesoscopic materials, which possess intrinsically nonlinear properties [lithium niobate (LiNbO3), bismuth germanium oxide (Bi12GeO20; BGO), bismuth silicon oxide (Bi12GeO20; BSO)], which have a nonzero electric susceptibility of the third order, χ(3)≠0. Corroborated Raman and coherent backscattering studies demonstrate that the occurrence of both effects is conditioned by the existence of a mesoscopic morphology of the sample, which is able to ensure efficient transport of the light inside the sample through a multiple light scattering mechanism. In this context, both AASRE and coherent backscattering effects are because of the Anderson localization of the light.
In this paper, we demonstrate that, by continuous single beam excitation, one can generate an abnormal anti-Stokes Raman emission (AASRE) whose properties are similar to a coherent anti-Stokes Raman scattering (CARS). The effect has been observed in materials which possess intrinsically nonlinear properties (LiNbO3 and CdS), which have the electric susceptibility of third order different from zero, χ(3) ≠ 0, as well as in materials that become nonlinear under resonant optical excitation. In the latter case, we used poly-3,4-ethylendioxythiophene (PEDOT) in its undoped state deposited electrochemically on Au support. Raman studies corroborated with images of optical microscopy demonstrate that the production of AASRE is conditioned by the existence of a particular morphology of the sample able to ensure efficient transport of the light inside the sample through a multiple light scattering mechanism. In this context, it was found that LiNbO3 and CdS in powder form as well as the PEDOT films layered on a rough Au substrate are suitable morphological forms. We explain AASRE as resulting from a wave-mixing mechanism of the incident laser light ωl with a Stokes-shifted Raman light ωS produced by a spontaneous Raman light scattering process, both strongly scattered inside the sample. As a CARS process, AASRE is conditioned by the achievement of phase-matching requirements, which makes the difference between the wave vectors of mixing light close to zero, Δk =/2kl − kS − kCARS/≈ 0. In condensed media, the small dispersion of the refractive index makes Δk ≈ 0 so that the formation of a favourable phase-matching geometry may be accomplished even at a crossing angle θ of travelling scattered light ωl and ωS. For tightly focused beams, the requirement of phase matching relaxes; it is no longer sensitive to the Raman shift, so that a wide intense anti-Stokes Raman spectrum is observed at an angle larger than the Stokes Raman spectrum.
It is known that spontaneous Raman scattering is accompanied by the appearance of nonclassical cross correlations of photons at Stokes and anti-Stokes frequencies. Such correlations occur due to the internal nonlinear interaction between electronic and nuclear vibration degrees of freedom. Since the properties of a given media are unchangeable, the possibilities for controlling the cross correlations are limited. This, in turn, restricts the possible applications of the correlated light obtained during the spontaneous Raman scattering. In this work, we investigate the influence of statistical properties of an incident light on the cross correlations of Stokes and anti-Stokes light. We show that the incoherence of the incident light results not only in the incoherence of the scattered light but also in the enhancement of the interbeam coherence at different frequencies. We demonstrate that the cross correlations of Stokes and anti-Stokes light intensities are enhanced when the incident light with high second-order autocorrelation function is applied. Our results pave the way to control correlated light obtained in the process of spontaneous Raman scattering.
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.
This manuscript presents a selection of works on the coherent evolution of atomic matter waves in random potentials. In this context, a number of interference, « mesoscopic » phenomena surviving a disorder average are discussed, in particular in the regime where Anderson localization shows up: coherent backscattering, coherent forward scattering, mesoscopic echo and quantum boomerang effect. The interplay between weak atomic interactions and Anderson localization is also touched upon for spreading wave packets, a scenario frequently considered in experiments. The last chapter, finally, gives an overview of recent works by the author on multiple scattering of light in media of dimension « (2+1) ». These peculiar systems, originally introduced to demonstrate Anderson localization of light in 2D, have sparked a growing interest in the recent years, for light propagation is governed by an effective Schrödinger equation and thus mimics the behavior of a matter wave. We here show that when the vector character of light is properly taken into account, these systems in fact display a physics much richer than the one pertained to this sole analogy.
We theoretically investigate ground-state depletion for subdiffraction-limited spatial resolution in coherent anti-Stokes Raman scattering (CARS) microscopy. We propose a scheme based on ground-state depopulation, which is achieved via a control laser light field incident prior to the CARS excitation light fields. This ground-state depopulation results in a reduced CARS signal generation. With an appropriate choice of spatial beam profiles, the scheme can be used to increase the spatial resolution. Based on the density matrix formalism we calculate the CARS signal generation and find a CARS signal suppression by 75% due to ground-state depletion with a single control light field and by using two control light fields the CARS signal suppression can be enhanced to 94%. Additional control light fields will enhance the CARS suppression even further. In case of a single control light field we calculate resulting CARS images using a computer-generated test image including quantum and detector noise and show that the background from the limited CARS suppression can be removed by calculating difference images, yielding subdiffraction-limited resolution where the resolution achievable depends only on the intensity used.