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Journal of Lightwave Technology

Spontaneous emission of dye molecules, semiconductor nanocrystals, and rare-earth ions in opal-based photonic crystals

Sergey V. Gaponenko, V. N. Bogomolov, Eugene P. Petrov, А. М. Капитонов, D.A. Yarotsky, I. I. Kalosha, Alexander Eychmueller, Andrey L. Rogach, John F. McGilp, U. Woggon, F. Gindele

Published Jan 1, 1999• 86 citations
Publisher

Abstract

Photonic crystals based on silica colloidal crystals (artificial opals) exhibit pronounced stopbands for electromagnetic wave propagation and the corresponding modification of the photon density of states in the visible range. These spectrally selective features can be enhanced by impregnating opals with higher refractive materials like, e.g., polymers. Doping of these structures with dye molecules, semiconductor nanoparticles (quantum dots), and rare-earth ions provides a possibility to examine the challenging theoretical predictions of the inhibited spontaneous emission in photonic bandgap (PBG) materials. First experiments are discussed in which pronounced modification of spontaneous emission spectra and noticeable changes in decay kinetics were observed.

DOI
10.1109/50.803003

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Physical Review A•Dec 13, 2000•99 citations
Photonic crystals based on silica colloidal crystals (artificial opals) exhibit pronounced stopbands for electromagnetic wave propagation and the corresponding modification of the photon density of states in the visible range. These spectrally selective features can be enhanced by impregnating opals with higher refractive materials like, e.g., polymers. Doping of these structures with dye molecules, semiconductor nanoparticles (quantum dots), and rare-earth ions provides a possibility to examine the challenging theoretical predictions of the inhibited spontaneous emission in photonic bandgap (PBG) materials. First experiments are discussed in which pronounced modification of spontaneous emission spectra and noticeable changes in decay kinetics were observed.
Chapter 1 IntroductionUltimate inhibition of spontaneous emission can be achieved in artificial periodic structures with tailor-made forbidden frequency bands [5].These periodic structures known as photonic crystals consist of different dielectric materials, where the index of refraction varies on length scales comparable to the wavelength of light.Therefore, the periodicity of photonic crystals is about 1000 times as large as that of atomic crystals.Light with specific frequencies is forbidden to propagate along certain directions by wave interference, similarly to Bragg diffraction of x-rays in atomic crystals.Such forbidden frequency ranges are called stopgaps.The larger the contrast of the refractive index between the two materials of a photonic crystal, the more strongly light is influenced, and the broader the stopgaps become.It was predicted in 1987 that an extreme situation may be feasible when light cannot propagate along any direction [6, 7].This situation is called a photonic bandgap.Spontaneous emission is completely inhibited for frequencies inside such a bandgap and, conversely, strongly enhanced for frequencies outside the bandgap.Photonic crystals, therefore, provide an ultimate tool for manipulating with light, which is of extreme interest for scientists and engineers [8, 9].Recent advances in nanotechnology have resulted in ability to synthesize semiconductor structures with dimensions of a few nanometers.Due to the finite sizes, electron-hole pairs (excitons) can be confined in these nanostructures, which leads to discrete excitonic energy levels.The nanocrystals that confine excitons in spherical or circular spaces are known as quantum dots.The discrete structure of the energy levels results in advantageous optical properties of these nanocrystals: narrow and tunable emission spectra.The emission frequencies can be tuned by varying the nanocrystal size: the smaller the size, the higher the emission frequency.These properties make the nanocrystals very promising elementary emitters for new experiments and devices [10, 11]. Outline of the thesisThis thesis describes time-and angle-resolved experiments, in which effects of threedimensional (3D) photonic crystals on spontaneous emission of embedded light sources (quantum dots and dye molecules) were studied.The thesis is organized as follows:In Chapter 2 we review the theoretical basics of the interaction between light and matter.We discuss the factors triggering the process of spontaneous emission and consider in detail the time evolution of the excited state of the emitter that interacts with the quantized 1.
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.
Photonic crystals, i.e. materials that have a periodic variation in refractive index, form an interesting new class of materials that can be used to modify spontaneous emission and manipulate optical modes in ways that were impossible so far. This thesis is divided in three parts. \nPart I discusses the design and fabrication of two-dimensional photonic crystals in silicon using deep anisotropic etching with a SF6/O2 plasma. The etching process was optimized for the fabrication of two-dimensional photonic crystals by tuning the main parameters of the etching process, i.e. temperature, bias voltage and O2 flow. Vertical confinement in these structures is provided by integrating the structures in a dielectric waveguide. For this purpose, amorphous silicon, silicon-on-insulator and SiGe structures were considered. Fabrication of structures in both amorphous silicon and silicon-on-insulator was successfully demonstrated. The incorporation of luminescent species, such as laser dyes, was demonstrated using a new wet chemical coating technique that forms thin silica layers on a substrate.\nPart II discusses the modification of spontaneous emission in one dimensional systems by studying the decay rate of luminescing Cr ions close to a dielectric interface. The decay rate of the Cr ions can be changed by bringing the samples into contact with a range of liquids with different refractive indices. The change in radiative decay rate can be calculated by calculating the local density of states. To explain the experimental results additional non-radiative decay channels have to be introduced and yields a quantum efficiency of ~50% for the Cr R-line luminescence. This concept was further extended to a thin silica layer on silicon implanted with erbium ions and resulted in the radiative rate of erbium in pure silica: 54 s-1. This number was used to analyze the decay rate of erbium ions in silica colloidal spheres that can be used as building block for three-dimensional photonic crystals by self-assembly.\nFinally, Part III discusses the optical properties and modified spontaneous emission from a three-dimensional silicon photonic crystal of finite (5-layers) thickness. The crystals are made in a layer-by-layer approach using lithographic tools and show near 100% reflection in the 1.4-1.7 mu m wavelength range indicative of a photonic stopgap. A direct comparison with the calculated reflectivity reveals that some features in the reflectivity can be ascribed to the finite thickness of the crystal, while other features can be explained in terms of a superstructure that leads to zone folding of the photonic bandstructure. The collected spontaneous emission from erbium implanted crystals is strongly reduced for wavelengths in the stopgap from 1.4-1.7 mu m. The changes in collected luminescence intensity are explained in terms of a rate equation model that takes into account the effect of Bragg scattering, the local density of states and the quantum efficiency of the emitters inside the crystal. Using this model a spectral attenuation of 5 dB per unit cell at 1.539 mu m wavelength is obtained from the experimental data, which is in perfect agreement with existing theory and transmission data.
We present the first experiments that demonstrate strong angle-independent modification of spontaneous emission spectra from laser dyes in photonic crystals, made of inverse opals in titania. We show that both the fluorescence quantum efficiency and weak disorder play a key role in interpreting the experimental data. We compare the angle-independent emission spectra of dye in photonic crystals with spectra from such crystals with much smaller lattice spacings, for which emission is in the long wavelength limit. The ratio of emission power spectra shows inhibition of emission up to a factor ∼ 5 over a large bandwidth of 13% of the first order Bragg resonance frequency. The inhibition shifts to increasing wavelength with the lattice parameter, confirming the photonic nature of the phenomenon. The center frequency and bandwidth of the inhibition agree with the calculated total density of states, but the measured inhibition of the vacuum fluctuations is much larger. This result is confirmed by experiments using different dyes. We likely probe the strongly modulated local photonic density of states, due to the spatially nonuniform distribution of dye molecules over the unit cell.
We have observed strongly modified spontaneous-emission spectra from laser dye in photonic crystals made of inverse opals in titania (TiO2).({\mathrm{TiO}}_{2}).(TiO2​). We identify stop bands with large relative widths of 1515%,15 comparable to the dyes' emission spectrum, and 7575%75 attenuation of the emission strength. For a wide range of angles, two stop bands are simultaneously manifested; their angle-dependent frequencies display an avoided crossing that is corroborated by reflectivity experiments. The edges of the stop bands agree well with band-structure calculations, but differ from simple Bragg diffraction as a result of multiple wave coupling. The strongly reduced dispersion of the Bloch modes likely causes a significant change in the density of states.