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Frontiers of Optoelectronics

Local density of states in photonic crystal cavity

Peng Qiu, Guang‐Long Wang, Jianglei Lu, Hongpei Wang

Published Jul 31, 2012• 3 citations
Publisher

Abstract

Local radiative density of optical states (LDOS) offers a tool to control the radiative rate of spontaneous emission from molecules, atoms, and quantum dots, which is proportional to LDOS. This paper presents that LDOS how to make the population of excited-state decay exponentially in time, and how these dynamics can be affected. By adopting the plane-wave expansion method, properties of an inverse-opal photonic crystal are studied with the help of photonic dispersion relations. Results in this paper show that the LDOS is radically modified in photonic crystal, and the rate of spontaneous emission can be described by the functions of position in the crystal and orientation of transition dipole moment.

DOI
10.1007/s12200-012-0271-0

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Local radiative density of optical states (LDOS) offers a tool to control the radiative rate of spontaneous emission from molecules, atoms, and quantum dots, which is proportional to LDOS. This paper presents that LDOS how to make the population of excited-state decay exponentially in time, and how these dynamics can be affected. By adopting the plane-wave expansion method, properties of an inverse-opal photonic crystal are studied with the help of photonic dispersion relations. Results in this paper show that the LDOS is radically modified in photonic crystal, and the rate of spontaneous emission can be described by the functions of position in the crystal and orientation of transition dipole moment.
Quantum electrodynamics of atom spontaneous emission from a three-dimensional photonic crystal is studied in a full vectorial framework. The electromagnetic fields are quantized via solving the eigenproblem of photonic crystals with use of a plane-wave expansion method. It is found that the photon density of states and local density of states (LDOS) with a full band gap vary slowly near the edge of band gap, in significant contrast to the singular character predicted by the previous isotropic model. Therefore, the spontaneous emission can be solved by conventional Weisskopf-Wigner approximate theory, which yields a pure exponentially decaying behavior with a rate proportional to the LDOS.
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.
Abstract We provide a pedagogical introduction to the concept of the local density of optical states (LDOS), illustrating its application to both the classical and quantum theory of radiation. We show that the LDOS governs the efficiency of a macroscopic classical antenna, determining how the antenna’s emission depends on its environment. The LDOS is shown to similarly modify the spontaneous emission rate of a quantum emitter, such as an excited atom, molecule, ion, or quantum dot that is embedded in a nanostructured optical environment. The difference between the number density of optical states, the LDOS, and the partial LDOS is elaborated and examples are provided for each density of states to illustrate where these are required. We illustrate the universal effect of the LDOS on emission by comparing systems with emission wavelengths that differ by more than 5 orders of magnitude, and systems whose decay rates differ by more than 5 orders of magnitude. To conclude we discuss and resolve an apparent difference between the classical and quantum expressions for the spontaneous emission rate that often seems to be overlooked, and discuss the experimental determination of the LDOS.
The dynamical characteristics of the spontaneous decay of a single excited atom or molecule depend strongly on its position within a photonic crystal (PC) and the relative orientation of its dipole and the electric field there. Measuring its dynamical characteristics of the spontaneous decay in a PC can only obtain the local density of states (DOS) in the PC, but cannot reflect the total DOS in the PC. It is found, theoretically, that using different number density distributions of luminescent molecules within the PC, one can probe the partial information or even all of the total DOS in the PC. In this paper, we separate, for the first time to our knowledge, the total DOS into two parts, DOS in the scatterer and DOS in the matrix of the Wigner-Seitz unit cell, according to their origin, and demonstrate that a special number density distribution of fluorescent molecules can reflect the total scatterers DOS or total matrix DOS or even both of them, i.e. the total DOS in the PC. This is meaningful in explaining and designing the experiments of prohibiting and enhancing the spontaneous emission of excited molecules.
Being motivated by the controversial results based on two dispersion models and Weisskopf–Wigner approximation (WWA), we introduce, for the first time to our knowledge, the position-dependent photon-atom interaction into the Green function method of the evolution operator and develop a universal theoretical approach to study spontaneous emission of atoms in photonic crystals (PCs). A position-sensitive generalized Lorentzian formalism (non-Lorentzian shape) for the decay of an excited atom in PCs is derived, and an exact numerical method for calculating the local coupling strength, proportional to the photonic local density of state (LDOS), is presented. For weak interaction PCs with pseudo gaps, the generalized Lorentzian formalism may be reduced to the famous Lorentzian spectrum. In this case, we introduce a lifetime distribution function for an assembly of atoms and find that it depends strongly on the atomic configuration in space, which clarifies successfully the tremendous discrepancy between different experiments. For the PCs with large full gaps, we find that the atomic position can fundamentally change the decay behavior of an excited atom: in strong interaction positions, the atomic decay is non-classical or exhibits an envelope-damped Rabi oscillation, while in weak interaction positions the WWA is valid. Recently, we also predicted giant Lamb shifts for hydrogen atoms in PCs, and revealed that in inhomogeneous electromagnetic environment, the dominant contribution to the Lamb shift comes from real photon emission, while the contribution from emission and reabsorption of virtual photon is negligible, in vast contrast with the case of free space where the virtual photon processes play a key role.