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Quantum Electronics

Speckle spectroscopy of fluorescent randomly inhomogeneous media

Dmitry A. Zimnyakov, I.A. Asharchuk, Sergey A. Yuvchenko, Аlexander P. Sviridov

Published Nov 9, 2016• 1 citation
Publisher

Abstract

We propose a coherence optical method for probing fluorescent randomly inhomogeneous media based on the statistical analysis of spatial fluctuations of spectrally selected fluorescence radiation. We develop a phenomenological model that interrelates the flicker index of the spatial distribution of the fluorescence intensity at a fixed wavelength and the mean path difference of partial components of the fluorescence radiation field in the probed medium. The results of experimental approbation of the developed method using the layers of densely packed silicon dioxide particles saturated with the aqueous rhodamine 6G solution with a high concentration of the dye are presented. The experimentally observed significant decrease in the flicker index under the wavelength tuning from the edges of the fluorescence spectrum towards it central part is presumably a manifestation of spectrally dependent negative absorption in the medium.

DOI
10.1070/qel16193

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We propose a coherence optical method for probing fluorescent randomly inhomogeneous media based on the statistical analysis of spatial fluctuations of spectrally selected fluorescence radiation. We develop a phenomenological model that interrelates the flicker index of the spatial distribution of the fluorescence intensity at a fixed wavelength and the mean path difference of partial components of the fluorescence radiation field in the probed medium. The results of experimental approbation of the developed method using the layers of densely packed silicon dioxide particles saturated with the aqueous rhodamine 6G solution with a high concentration of the dye are presented. The experimentally observed significant decrease in the flicker index under the wavelength tuning from the edges of the fluorescence spectrum towards it central part is presumably a manifestation of spectrally dependent negative absorption in the medium.
Stochastic interference of partially coherent light multiple scattered by a random medium is considered. The relationship between the second- and third-order moments of intensity fluctuations in random interference patterns, the coherence function of probe radiation, and the probability density of path differences for the interfering partial waves in the medium are established. The obtained relationships were verified using the statistical analysis of spectrally selected fluorescence radiation emitted by the laser-pumped dye-doped random medium. Rhodamine 6G water solution was applied as the doping agent for the ensembles of densely packed silica grains which were pumped by the CW radiation (532 nm) from the diode-pumped solid state laser. Experimentally observed abrupt decay of the second- and third-order moments of fluorescence intensity fluctuations for the wavelengths ranging from 620 nm to 680 nm is interpreted in terms of amplification of spontaneous emission at large dye concentrations. This paper discusses the new optical probe of random media defined as "the reference-free path length interferometry with the intensity moments analysis".
The saturation of the spectral quality of the fluorescence response of randomly inhomogeneous media to external laser pump with intensities above the random lasing threshold in a medium has been studied. It has been found that the saturation of the fluorescence spectral quality is due to a decrease in the fluorescence enhancement length in the medium to the minimum value determined by the average size of local fluorescence emitters associated with laser speckles and by radiative exchange between emitters.
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.
This paper presents a review of research, both theoretical and experimental, concerning the influence of coherence properties of fluctuating light sources and of correlation properties of scattering media on the spectra of radiated and scattered fields. Much of this research followed a discovery made in 1986, that the spectrum of light may change on propagation, even in free space. More than 100 papers on this topic have been published to date and many of them are reviewed, or at least mentioned, in this article. After an introduction and a summary of some of the main mathematical results relating to second-order coherence theory of statistically stationary optical fields, spectral changes that may take place on superposing fields produced by two partially correlated sources are discussed. Spectral effects in fields produced by two-dimensional secondary sources and by three-dimensional primary sources are then considered. The section which follows describes spectral changes that may arise when polychromatic light is scattered on media whose physical properties vary randomly either in space and/or in time. A review is also presented of recent research, which has revealed that under certain circumstances the changes in the spectrum of light scattered on random media may imitate the Doppler effect, even though the source, the medium and the observer are all at rest with respect to one another. In the final section a brief review is given of a new emerging technique sometimes called spatial-coherence spectroscopy. It is based on the discovery that it is possible, under certain circumstances, to determine field correlations from spectral measurements.
The approximation of small fluctuations of the optical field is used to solve the transient problem of conversion of the spatial statistics of partly coherent radiation in a randomly inhomogeneous weakly absorbing medium. Pulsed radiation is considered and it is assumed that the pulse duration does not exceed the lifetime of inhomogeneities. Equations derived for the coherence functions of field perturbations are used to study in detail the dynamics of the statistical characteristics of radiation, such as the correlation radius, variance of the fluctuations, correlation functions of the amplitudes, and phase of the field perturbations.
Abstract Based on the analysis of experimental data on the effect of the pulsed laser pump intensity on the spectral properties and the size of the fluorescent response zone in randomly inhomogeneous fluorescent layers, we found that the amplification of spontaneous and stimulated emission significantly affects the statistical properties of the propagation lengths of the fluorescent field partial components in the layers. The experiments are performed with layers of SiO2 and TiO2 nanoparticles saturated with rhodamine 6G, pumped by 532-nm laser radiation in the intensity range corresponding to the transient regime from excitation of spontaneous fluorescence to random lasing in the layer. The experimental data are compared with the results of statistical modelling of fluorescence transfer. It is shown that, even at a pump intensity below the random lasing threshold, the spontaneous emission amplification in a layer leads to a significant increase in the contributions to the fluorescence response from partial components with propagation lengths much larger than the layer thickness. This can be interpreted as a manifestation of the quasi-waveguide effect, in which the probability of propagation of diffuse fluorescence components along the layer over distances many times greater than its thickness and the size of the pumped region increases significantly with a decrease in the characteristic radiation amplification length in the layer.