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Acta Physica Polonica A

Modification of the Spontaneous Emission of Dye Molecules in Photonic Crystals

Eugene P. Petrov, V. N. Bogomolov, I. I. Kalosha, Sergey V. Gaponenko

Published Nov 1, 1998• 9 citations
Publisher

Abstract

Modification of the spontaneous emission of dye molecules embedded in artificial opals exhibiting stop bands in the visible range is observed.Molecules embedded in artificial opals show dips in spontaneous emission spectra and modified fluorescence decay kinetics.Results are interpreted in terms of redistribution of the photon density of states.Effects of the multiple reabsorption and reemission of fluorescence photons and interaction of dye molecules with the silica surface are discussed.

DOI
10.12693/aphyspola.94.761

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Modification of the spontaneous emission of dye molecules embedded in artificial opals exhibiting stop bands in the visible range is observed.Molecules embedded in artificial opals show dips in spontaneous emission spectra and modified fluorescence decay kinetics.Results are interpreted in terms of redistribution of the photon density of states.Effects of the multiple reabsorption and reemission of fluorescence photons and interaction of dye molecules with the silica surface are discussed.
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 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.
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.
The photonic dispersion, the group-velocity dispersion, the effective mass, refractive index, and the spectral distribution of the density of photonic states near the edge of the photonic stop band are numerically calculated in the one-dimensional model for photonic crystals based on synthetic opals. The fluorescence spectra of rhodamine 6G and 2,5-bis(2-benzoxazolyl)hydroquinone molecules infiltrated into a synthetic opal are measured. For both substances, it is observed that the spontaneous emission intensity in the range of the photonic stop band is appreciably suppressed. A blue shift of the fluorescence spectrum of rhodamine 6G molecules is revealed. Secondary emission of synthetic opals infiltrated with colloidal silver is observed in the Stokes range under excitation of opals by radiation at λ = 400 nm. The spectrum of the secondary emission is located in the range 450–590 nm, which contains the stop band and intervals near its edges.