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Optics Letters

Spectral measurements of the emission from highly scattering gain media

G. Beckering, Stephan J. Zilker, D. Haarer

Published Sep 15, 1997• 42 citations
Publisher

Abstract

The spectral properties of the emission of a colloidal suspension of titanium dioxide particles in Rhodamine 640 perchlorate were studied systematically. The particle density rho, the dye concentration c, and the energy of the pump pulse were varied over several orders of magnitude; the dependence of the spectra on these three parameters is discussed. We discovered a strong correlation between the particle density and the dye concentration. The amplification by stimulated emission was found to be strongest when the absorption length l(a) and the mean-free-path length l(*) had approximately the same magnitude. The respective l(*) values were determined by a pulsed transmission experiment.

DOI
10.1364/ol.22.001427

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The spectral properties of the emission of a colloidal suspension of titanium dioxide particles in Rhodamine 640 perchlorate were studied systematically. The particle density rho, the dye concentration c, and the energy of the pump pulse were varied over several orders of magnitude; the dependence of the spectra on these three parameters is discussed. We discovered a strong correlation between the particle density and the dye concentration. The amplification by stimulated emission was found to be strongest when the absorption length l(a) and the mean-free-path length l() had approximately the same magnitude. The respective l() values were determined by a pulsed transmission experiment.
In several recent experiments, isotropic lasing action was observed in paints that contain rhodamine 640 dye molecules in methanol solution as gain media and titania particles as optical scatterers. These so-called paint-on laser systems are extraordinary because they are highly disordered systems. The microscopic mechanism for laser activity and the coherence properties of light emission in this multiple-light-scattering medium have not yet been elucidated. In this paper we derive the emission intensity properties of a model dye system with excited singlet and triplet electronic energy levels, which is immersed in a multiple-scattering medium with transport mean free path l*. Using physically reasonable estimates for the absorption and emission cross section for the singlet and triplet manifolds, and the singlet-triplet intersystem crossing rate, we solve the nonlinear laser rate equations for the dye molecules. This leads to a diffusion equation for the light intensity in the medium with a nonlinear intensity-dependent gain coefficient. Using this model we are able to account for nearly all of the experimentally observed properties of laser paint reported so far when l*\ensuremath{\gg}${\ensuremath{\lambda}}_{0}$, the emission wavelength. This includes the dependence of the peak intensity of amplified emission on the mean free path l*, the dye concentration \ensuremath{\rho}, and the pump intensity characteristics. Our model recaptures the collapse of the emission linewidth at a specific threshold pump intensity and describes how this threshold intensity varies with l*. In addition, our model predicts a dramatic increase in the peak intensity and a further lowering of the lasing threshold for the strong scattering limit l*\ensuremath{\rightarrow}${\ensuremath{\lambda}}_{0}$. This suggests a striking enhancement of the characteristics of laser paint near the photon localization threshold in a disordered medium. \textcopyright{} 1996 The American Physical Society.
The features of fluorescence emission in a dye-doped dense multiple scattered medium under pulsed laser pumping are considered in terms of confined excitation in small zones associated with laser speckles occurring in a pumped medium. The results of numerical modeling of the fluorescence emission kinetics are compared to the experimental data obtained using the rhodamine 6G-doped layers of the densely packed TiO2 (anatase) particles pumped at 532 nm by 10 ns laser pulses. The intensity of pump radiation during the action of laser pulses was varied from 1·105 W/cm2 to 5·107 W/cm2. In the recovery of the ratios of stimulated to a spontaneous emission, the spectra of the stimulated component were fitted using the spectral function derived by R. Dicke. In the framework of the considered concept, saturation of the ratio of the stimulated to a spontaneous emission and linear growth of an integrated fluorescence output with a practically unchangeable half-width of the emission spectra at high pump intensities are interpreted.
We report enhanced emission and gain narrowing in Rhodamine 590 perchlorate dye in an aqueous suspension of polystyrene microspheres. A systematic experimental study of the threshold condition for and the gain narrowing of the stimulated emission over a wide range of dye concentrations and scatterer number densities showed several interesting features, even though the transport mean free path far exceeded the system size. The conventional diffusive-reactive approximation to radiative transfer in an inhomogeneously illuminated random amplifying medium, which is valid for a transport mean-free path much smaller than the system size, is clearly inapplicable here. We propose a new probabilistic approach for the present case of dense, random, weak scatterers involving the otherwise rare and ignorable sub-mean-free-path scatterings, now made effective by the high gain in the medium, which is consistent with experimentally observed features.
Emission spectra of concentrated (~10 18 –10 19 cm –3 ) ethanol solutions of Rhodamine C excited by high-power (~10 25 –10 26 cm –2 s –1 ) laser radiation were measured. The emission spectrum consists of two narrow bands (with half-widths of ~200–300 cm –1 ). The long-wavelength band was interpreted as cooperative spontaneous emission, and the short-wavelength band was assigned to the amplified spontaneous emission. The ratio of their intensities depends on the dye concentration and the pump power density. The ratio of band intensities is assumed to be determined by the dephasing rate of excited molecules responsible for cooperative spontaneous emission.
We experimentally examined the threshold of the spectral collapse in dye embedded in a strongly scattering medium as a function of the excitation beam diameter and the transport mean free path in order to find a condition to minimize the threshold. We found a critical transport mean free path, below which the threshold pulse energy is almost independent of the mean free path. Experimental observations are well explained by a theoretical model based on the rate and diffusion equations, which shows that the luminescence spectra are also dependent on the position in the medium.