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Frontiers in Optics

Coupling of random lasing and stimulated Raman scattering in a random media: Necessary conditions

Vasil P. Yashchuk, A.P. Smaliuk, Eugene A. Tikhonov

Published Jan 1, 2020• 1 citation
Publisher

Abstract

Random lasing (RL) in disordered active media can initiate stimulated Raman Scattering (SRS). We have found the optimal condition of SRS-RL coupling, which is perspective for Raman spectroscopy applications.
DOI
10.1364/fio.2020.jth4a.35

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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 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.
A theory of stimulated Raman scattering (SRS) is presented which treats in a unified manner the buildup of SRS from spontaneous Raman scattering and the spatial propagation which leads to gain. Maxwell-Bloch equations describe the coupling between the Stokes field operator and the collective atomic operators, which are driven by a classical laser field under low-signal-gain conditions, where the atomic ground states and laser field remain undepleted. An analytic expression is derived for the forward-propagating Stokes field operator in a one-dimensional spatial approximation when the Fresnel number of the excited medium is unity. Steady-state and transient Stokes intensities are evaluated under low-gain (spontaneous) and high-gain (stimulated) conditions. The Stokes intensity is found to be exactly independent of a laser bandwidth arising solely from phase fluctuations. The power spectrum of steady-state SRS is evaluated, giving a gain-narrowed spectral profile when the laser is narrow band, and a spectrum identical to the laser spectrum when the laser is broad band. A strong analogy between SRS and two-level superfluorescence is found; in both cases the macroscopic, collective dipole moment is initiated by quantum fluctuations.
Stimulated Raman scattering (SRS) microscopes are a standard technique to image cells, tissues or track the uptake of drugs [1] . The sensitivity in these devices is directly linked to the laser power. While an increase of sensitivity is desired, increasing the laser power is challenging and squeezed light offers a solution to this challenge. Recently squeezed light has been used to enhance the sensitivity of continuous-wave and pulsed SRS [2] , [3] setups and stimulated emission spectroscopy [4] .
Recently, competing random lasing and stimulated Raman scattering mechanisms have been observed for the same gain medium infiltrated in diffusive silica‐based solid foams. Specifically, the light transport mean free path in such disordered media has been identified to be a parameter of choice to tune the observation of either Raman or random lasing. In this contribution, novel silica‐/titania‐based solid foams are designed that allow tuning this parameter significantly, by one order of magnitude. This being achieved, the transition from “pure” random to “pure” Raman lasing is shown, while going through a state of concomitant existence of both mechanisms. The experimental results are well understood, owing to simulations of a simple 1D diffusive model, which suggests that both gain mechanisms may present a complex interplay, leading to random Raman lasing.