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ACS Photonics

Disorder as a Playground for the Coexistence of Optical Nonlinear Effects: Competition between Random Lasing and Stimulated Raman Scattering in Complex Porous Materials

Nicolas Bachelard, Preeti Gaikwad, Rénal V. Backov, Patrick Sebbah, Renaud A. L. Vallée

Published Oct 14, 2014• 28 citations
Publisher

Abstract

We predict the coexistence and competition of random lasing and stimulated Raman scattering (SRS) in active disordered random media. We develop a simple model that includes both mechanisms coupled to diffusion equation. We find that the prevalence of a nonlinear mechanism over the other is determined by the degree of scattering. This is confirmed experimentally in dye-infiltrated three-dimensional porous silica-based disordered samples, with controllable pore size and transport properties. Experimentally, random lasing dominates in a sample with a large transport mean free path, l t ≈ 100 μm, while it gives way to SRS for l t ≈ 25 μm. The competition is explained in terms of disorder-dependent pump depletion and fluorescence saturation.

DOI
10.1021/ph500280m

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We predict the coexistence and competition of random lasing and stimulated Raman scattering (SRS) in active disordered random media. We develop a simple model that includes both mechanisms coupled to diffusion equation. We find that the prevalence of a nonlinear mechanism over the other is determined by the degree of scattering. This is confirmed experimentally in dye-infiltrated three-dimensional porous silica-based disordered samples, with controllable pore size and transport properties. Experimentally, random lasing dominates in a sample with a large transport mean free path, l t ≈ 100 μm, while it gives way to SRS for l t ≈ 25 μm. The competition is explained in terms of disorder-dependent pump depletion and fluorescence saturation.
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Random lasing (RL) and stimulated Raman scattering (SRS) of dye in multiple scattering media (MSM) appears simultaneously and each couple with other. This coupling has considerable influence on the SRS regularities of dye in MSM. The main feature of this impact is that RL radiation promotes the Raman lines revealing in the RL spectrum range as part of total radiation. SRS initiation occurs owing to the CARS-like mechanism provided by the two component pump: incident monochromatic radiation (laser pump) and RL radiation arising inside the MSM. It leads to important consequences: the RL spectrum must overlap with the spectral region of the possible Stokes lines of the dye; only those Stokes lines appear which are in a range of the RL spectrum; all conditions which promote RL assist SRS also. It is shown MSM promotes the best conditions for SRS and RL coupling due to optimal matching of RL localization regions and pump radiation.
We report on a medium exhibiting extremely efficient light scattering properties: a liquid network formed in a porous matrix. Liquid fragments confined in the solid matrix result in a random fluctuation of the dielectric function and act as scattering objects for photons. The optical scattering efficiency is defined by the filling factor of the liquid in the pores and its dielectric constant. The spectral dependence of the scattering length of photons indicates that the phenomenon is governed by a Mie-type scattering mechanism. The degree of the dielectric disorder of the medium, i.e. the level of opacity is tunable by the ambient vapor pressure of the dielectric substance. In the strongest scattering regime the scattering length of photons is found to be in the micrometer range. By incorporation of dye molecules in the voids of the porous layer a system exhibiting optical gain is realized. In the multiple scattering regime the optical path of diffusively propagating photons is enhanced and light amplification through stimulated emission occurs: a strong intensity enhancement of the dye emission accompanied by significant spectral narrowing is observed above the excitation threshold for a layer being in the opalescence state. (© 2005 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim)
The spatial formation of coherent random laser modes in strongly scattering disordered random media is a central feature in the understanding of the physics of random lasers. We derive a quantum field theoretical method for random lasing in disordered samples of complex amplifying Mie resonators which is able to provide self-consistently and free of any fit parameter the full set of transport characteristics at and above the laser phase transition. The coherence length and the correlation volume respectively is derived as an experimentally measurable scale of the phase transition at the laser threshold. We find that the process of stimulated emission in extended disordered arrangements of active Mie resonators is ultimately connected to time-reversal symmetric multiple scattering in the sense of photonic transport while the diffusion coefficient is finite. A power law is found for the random laser mode diameters in stationary state with increasing pump intensity.