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Physical Review Letters

Spontaneous emission in a disordered dielectric medium

Jordi Martorell, N. M. Lawandy

Published Feb 18, 1991• 34 citations
Publisher

Abstract

We observed the change in fluorescence lifetime from a molecular dye embedded in a colloidal suspension of polystyrene spheres when the mean separation between spheres remains less than the wavelength of emission. At high densities of colloidal particles the spontaneous emission is inhibited, while as the density of colloidal particles is lowered the spontaneous emission is enhanced. This phenomenon is interpreted in terms of coherent interference from the electric field radiated by the molecular dipole and the reradiated field from the dielectric spheres.

DOI
10.1103/physrevlett.66.887

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Acta Physica Polonica A•Nov 1, 1998•9 citations
We observed the change in fluorescence lifetime from a molecular dye embedded in a colloidal suspension of polystyrene spheres when the mean separation between spheres remains less than the wavelength of emission. At high densities of colloidal particles the spontaneous emission is inhibited, while as the density of colloidal particles is lowered the spontaneous emission is enhanced. This phenomenon is interpreted in terms of coherent interference from the electric field radiated by the molecular dipole and the reradiated field from the dielectric spheres.
Summary form only given. Over the last three decades of the 20 th century many experiments have demonstrated that the rate of spontaneous emission for an emitter is determined by its electromagnetic surrounding. This phenomenon has been usually studied for atoms or molecules placed in the vicinity of mirrors or in optical resonators. Furthermore, it is also well-known that the fluorescence lifetime of an emitter changes after being embedded in dielectric media where aside from a change in the refractive index, it experiences the local fields in the dielectric. For a spherical medium larger than the order of a wavelength it is known that the coupling to Mie modes of this dielectric resonator has a large influence on the emission rate of an emitter inside. However, when the medium becomes comparable or smaller than a wavelength one can no longer speak of resonator modes. Here we report on an experiment where we have studied the variation of the spontaneous emission rate as the dielectric medium surrounding an emitter is made smaller and smaller down to a few nanometers.
We measure fluorescence lifetimes of emitters embedded in isolated single dielectric nanospheres. By varying the diameters of the spheres from 100 nm to 2 microm and by modifying their dielectric surrounding, we demonstrate a systematic change of paradigm in the spontaneous emission rate, as we cross the border from the superwavelength regime of Mie resonances to the nanoscopic realm of Rayleigh scattering. Our data show inhibition of the spontaneous emission up to 3 times and are in excellent agreement with the results of analytical calculations.
Summary form only given. Over more than three decades many experiments have shown that the rate of spontaneous emission from an emitter can be strongly modified due to its electromagnetic surrounding. It is also well-known that the fluorescence lifetime of an emitter changes when embedded in dielectric media where aside from a change in the density of states, it is influenced by the local fields in the dielectric. The goal of our work has been to study the transition between the regime of an emitter in vacuum to that of a bulk dielectric medium, emphasizing the domain where the emitter's environment has a subwavelength extent. In our experiment we have investigated the dependence of the spontaneous emission rate of Eu/sup 3+/ ions in polymer nanospheres of different diameters, ranging from 20nm to 2000nm. In order to perform well-defined control experiments, we have combined atomic force microscopy and fluorescence confocal microscopy to make measurements only on isolated single spheres lying on a glass substrate.
We report on modification of the spontaneous emission of dye molecules embedded in a three-dimensional solid-state photonic crystal exhibiting a stop band in the visible range. Molecules embedded in artificial opal filled with a polymer show a dip in the fluorescence spectrum and nonexponential spontaneous decay kinetics containing both accelerated and inhibited components compared to the dye fluorescence in a reference polymer matrix. Results are interpreted in terms of redistribution of the photon density of states in the photonic crystal.