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Physical Review A

Theory of fluorescence in photonic crystals

Nipun Vats, Sajeev John, Kurt Busch

Published Mar 21, 2002• 202 citations
Publisher

Abstract

We present a formalism for the description of fluorescence from optically active materials embedded in a photonic crystal structure possessing a photonic band gap or pseudogap. An electromagnetic field expansion in terms of Bloch modes of the crystal is used to develop the equations for fluorescence in terms of the local density of photon modes available to the emitting atoms in either the high or low dielectric regions of the crystal. We then obtain expressions for fluorescence spectra and emission dynamics for luminescent materials in photonic crystals. The validity of our formalism is demonstrated through the calculation of relevant quantities for model photon densities of states. The connection of our calculations to the description of realistic systems is discussed. We also describe the consequences of these analyses on the accurate description of the interaction between radiative systems and the electromagnetic reservoir within photonic crystals.

DOI
10.1103/physreva.65.043808

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We present a formalism for the description of fluorescence from optically active materials embedded in a photonic crystal structure possessing a photonic band gap or pseudogap. An electromagnetic field expansion in terms of Bloch modes of the crystal is used to develop the equations for fluorescence in terms of the local density of photon modes available to the emitting atoms in either the high or low dielectric regions of the crystal. We then obtain expressions for fluorescence spectra and emission dynamics for luminescent materials in photonic crystals. The validity of our formalism is demonstrated through the calculation of relevant quantities for model photon densities of states. The connection of our calculations to the description of realistic systems is discussed. We also describe the consequences of these analyses on the accurate description of the interaction between radiative systems and the electromagnetic reservoir within photonic crystals.
In the first part of this introductory review we outline the developments in photonic band gap materials from the physics of photonic band gap formation to the fabrication and potential applications of photonic crystals. We briefly describe the analogies between electron and photon localization, present a simple model of a band structure calculation and describe some of the techniques used for fabricating photonic crystals. Also some applications in the field of photonics and optical circuitry are briefly presented. In the second part, we discuss the consequences for the interaction between an atom and the light field when the former is embedded in photonic crystals of a specific type, exhibiting a specific form of a gap in the density of states. We first briefly review the standard treatment (Weisskopf – Wigner theory) in describing the dynamics of spontaneous emission in free space from first principles, and then proceed by explaining the alterations needed to properly treat the case of a two-level atom embedded in a photonic band gap material.
A photonic crystal, defined as a periodic dielectric structure, can influence the radiation rate of an embedded dipolar emitter. A theory of this effect is developed and the efficiency of a dipolar photonic source is calculated for a realistic three-dimensional crystal. Taking as a starting point the photonic band structure and its associated eigenfields, it is shown that the emission rate is strongly correlated with the density of modes, but also that the density of modes alone cannot explain all features found in the emission spectrum. For an infinite crystal, the computation of the field propagator confirms that the emission rate falls to zero in the frequency range defined by the photonic band gap. The emitter lifetime changes with the dipole location and orientation, leading to a radiation rate enhancement or inhibition according to the direction of the emission. These results may open routes to photonic sources with very high quantum efficiency.
The radiation dynamics of a dipole antenna embedded in a photonic crystal are modeled by an initially excited harmonic oscillator coupled to a non-Markovian bath of harmonic oscillators representing the colored electromagnetic vacuum within the crystal. Realistic coupling constants based on the natural modes of the photonic crystal, i.e., Bloch waves and their associated dispersion relation, are derived. For simple model systems, well-known results such as decay times and emission spectra are reproduced. This approach enables direct incorporation of realistic band structure computations into studies of radiative emission from atoms and molecules within photonic crystals. We therefore provide a predictive and interpretative tool for experiments in both the microwave and optical regimes.
We present a formula to evaluate the spontaneous emission spectra of an atom in contact with a radiation field with non-Markovian effects. This formula is written in terms of a two-time correlation of system observables and the environmental correlation function, and depends on the distance between the emitting atom and the detector. As an example, we use it to analyze the fluorescence spectra of a two level atom placed as an impurity in a photonic crystal. The radiation field within those materials has a gap or discontinuity where electromagnetic modes cannot propagate in the stationary limit. In that situation, the atomic emission occurs in the form of evanescent waves which are detected with less efficiency the farther we place the detector. The methodology presented in this paper may be useful to study the non-Markovian dynamics of any quantum open system in linear interaction with a harmonic oscillator reservoir and within the weak-coupling approximation.
Photonic crystals affect the photon emission of embedded emitters due to an altered local density of photon states (LDOS). We review the calculation of the LDOS from eigenmodes in photonic crystals and propose a rate equation model for fluorescent emitters to determine the changes in emission induced by the LDOS. We show how to calculate the modifications of three experimentally accessible characteristics: emission spectrum (spectral redistribution), emitter quantum yield, and fluorescence lifetime. As an example, we present numerical results for the emission of the dye Rhodamine B inside an opal photonic crystal. For such photonic crystals with small permittivity contrast, the LDOS is only weakly modified, resulting in rather small changes. We point out that in experiments, however, usually only part of the emitted light is detected, which can have a very different spectral distribution (e.g., due to a photonic band gap in the direction of detection). We demonstrate the calculation of this detected spectrum for a typical measurement setup. With this reasoning, we explain the previously not fully understood experimental observation that strong spectral modifications occurred, while at the same time only small changes in lifetime were found. With our approach, the mentioned effects can be quantitatively calculated for fluorescent emitters in any photonic crystal.