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Physical review. B, Condensed matter

Theory of optical-environment-dependent spontaneous-emission rates for emitters in thin layers

W. Lukosz

Published Sep 15, 1980• 139 citations
Publisher

Abstract

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 ${d}_{0}$ 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 ${n}_{j}$ of media $j=0, 1, \mathrm{and} 2$ 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 ${\mathrm{Eu}}^{3+}$ ions in varying optical environments, which yielded the quantum efficiency of the emitting state.

DOI
10.1103/physrevb.22.3030

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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 n0d0\ensuremath≪\ensuremathλ8{n}_{0}{d}_{0}\ensuremath{\ll}\frac{\ensuremath{\lambda}}{8}n0​d0​\ensuremath≪8\ensuremathλ​ (where \ensuremathλ\ensuremath{\lambda}\ensuremathλ 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.
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.
The spontaneous decay rates of atoms can be altered by embedding them in a bulk dielectric medium. The alteration of the decay rates depends on three physical factors: a photon density of state factor, a local-field correction factor, and a field normalization factor. There are conflicting expressions in the literature for the local-field correction and field normalization factors. However, it is expected that for a thin slab a change in the total decay rate for an embedded atom or exciton should change when the slab thickness is approximately ( λ )/2πn. We are fabricating dielectric slabs with dimensions in this range that will allow us to demonstrate both the dependence of decay rate on the slab thickness and the index of the surrounding medium. Our experiment involves a technique for embedding thin GaAs/AlGaAs quantum well structures in different dielectric media with n ranging 1.5–3.5 and measuring the spontaneous decay rates.
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.
In this chapter, the author calculates the modification of the spontaneous emission pattems and the corresponding rate change using classical physics. To derive the spontaneous emission pattems or rates the readers must average the emission rate at each frequency over this distribution function. It is important to understand that this assumption is only valid if the emission line is homogeneously broadened (albeit not necessarily at its natural linewidth limit due to the radiative decay). One more thing needs to be pointed out before the readers move on to a more exact calculation of the spontaneous emission pattern and the emission rate of a dielectric cavity. In the ideal mirror the reflection takes place at a well-defined plane. Integration of the emission over all solid angles and all wavelengths gives us information about the total spontaneous emission rate, or, equivalently, about the spontaneous emission lifetime of an emitter in a dielectric cavity.
We consider the spontaneous emission in an absorbing medium by calculating the quantum flow of energy from an emitting atom. For this purpose, we extend the analysis by Power and Thirunamachandran of quantized Maxwell fields in the vicinity of an atom in the free space to a situation where the emitter is in a dielectric medium. We represent the quantum flow in terms of the non-equal time commutators involving electric and magnetic fields, as well as the local displacement field. The commutators are calculated applying a previously developed microscopic theory of quantization of radiation in dielectrics. Consequently, we derive from first principles the rate of spontaneous emission in an absorbing medium containing local field factors and other refractive contributions. The results support the previous introduction of the (virtual cavity) local field correction by Barnett et al on a phenomenological basis, as well as our previous approach in which the spontaneous emission is considered as a resonance energy transfer to the far-zone atoms. A distinctive feature of the present formalism is that it deals with the spontaneous emission directly by calculating the quantum flow from the emitting atom. Therefore, the method is free from divergences appearing in other approaches analysing the spontaneous decay in absorbing media.