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Quantum Electronics and Laser Science Conference

Spontaneous emission in nanoscopic media: Rayleigh scattering of vacuum fluctuations

Hannes C. Schniepp, Vahid Sandoghdar

Published Nov 13, 2002• 0 citations
Publisher

Abstract

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.

DOI
10.1109/qels.2001.961863

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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.
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.
The spontaneous-emission rates of emitters embedded in a thin layer 0 of a loss-free dielectric depend on their optical environment, i.e., on the optical properties of the two media 1 and 2 adjoining layer 0. For electric- and magnetic-dipole transitions the spontaneous-emission rates, normalized with respect to those in an infinite medium 0, are expressed in terms of the Fresnel reflection coefficients for plane and evanescent waves incident from medium 0 on the interfaces to the planar-stratified or homogeneous media 1 and 2, respectively. From this result which is valid for arbitrary layer thicknesses d0{d}_{0}d0​ we derive an approximation for extremely thin layers of optical thickness ${n}_{0}{d}_{0}\ensuremath{\ll}\frac{\ensuremath{\lambda}}{8}$ (where $\ensuremath{\lambda}$ is the emission wavelength) between two homogeneous loss-free dielectric media 1 and 2. For the normalized spontaneous-emission rates as functions of the refractive indices nj{n}_{j}nj​ of media j=0,1,and2j=0, 1, \mathrm{and} 2j=0,1,and2 analytical expressions are obtained. We have used these expressions previously without proof [Phys. Rev. B 21, 4814 (1980)] to analyze experimentally observed changes in the fluorescence lifetime of Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions in varying optical environments, which yielded the quantum efficiency of the emitting state.
In order to discriminate between the two macroscopic models for the dependence of the spontaneous emission rates of emitters on the refractive indices of the surrounding optical dielectric media, i.e., the local-field effect, Eu3+ activated glass samples with a range of different refractive indices were prepared for the measurements of photoluminescence emission spectrum, luminescent decay rate and refractive index. Detail analyses indicate that the local-field effect on the spontaneous emission rates follows the virtual-cavity model derived by assuming the doped luminescent ions do not disturb the optical dielectric media.
Fluorescence lifetimes of nitrogen-vacancy color centers in individual diamond nanocrystals were measured at the interface between a glass substrate and a strongly scattering medium. Comparison of the results with values recorded from the same nanocrystals at the glass-air interface revealed fluctuations of fluorescence lifetimes in the scattering medium. After discussing a range of possible systematic effects, we attribute the observed lengthening of the lifetimes to the reduction of the local density of states. Our approach is very promising for exploring the strong threedimensional localization of light directly on the microscopic scale.
The effect of the dielectric medium upon the spontaneous emission rate was investigated using lead borate glass of various compositions lightly doped with the Eu3+{}^{3+}3+ lanthanide ion. A dual approach used the variation of (i) electric dipole/magnetic dipole (ED/MD) emission rates from spectral integrations and (ii) absolute ED emission rates from lifetime measurements for comparison with the variation of the refractive index of the glass medium. Contrary to a previous study [Phys. Rev. Lett. 91, 203903 (2003)], the results show the relevance of the virtual-cavity model in this case. The MD emission rates were taken to follow the n3{n}^{3}n3 increase in density of photon states in the medium. The justifications for employing Eu3+{}^{3+}3+ for identifying the appropriate model are given.