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Physical Review Letters

Observation of inhibited spontaneous emission in a periodic dielectric structure

Jordi Martorell, N. M. Lawandy

Published Oct 1, 1990• 219 citations
Publisher

Abstract

Inhibition of the radiative decay of dye molecules embedded in an ordered aqueous suspension of polystyrene spheres has been measured using picosecond pump-probe techniques. The inhibition is interpreted in terms of excluded vacuum modes and compared with results based on the Wigner-Weisskopf formalism and a three-dimensional scattering model for the fcc colloidal structures.

DOI
10.1103/physrevlett.65.1877

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•May 21, 1990•0 citations
Inhibition of the radiative decay of dye molecules embedded in an ordered aqueous suspension of polystyrene spheres has been measured using picosecond pump-probe techniques. The inhibition is interpreted in terms of excluded vacuum modes and compared with results based on the Wigner-Weisskopf formalism and a three-dimensional scattering model for the fcc colloidal structures.
We observed the change in fluorescence lifetime from a molecular dye embedded in a colloidal suspension of polystyrene spheres when the mean separation between spheres remains less than the wavelength of emission. At high densities of colloidal particles the spontaneous emission is inhibited, while as the density of colloidal particles is lowered the spontaneous emission is enhanced. This phenomenon is interpreted in terms of coherent interference from the electric field radiated by the molecular dipole and the reradiated field from the dielectric spheres.
In 1946 Purcell showed that the spontaneous emission rate of an atomic system could be enhanced by placing it in a conducting cavity. Later, Kleppner showed that spontaneous emission could also be inhibited if the vacuum modes coupled to the atom were excluded by a structure. Most recently, we experimentally have shown that a periodic dielectric structure could alter the spontaneous emission by Bragg scattering of vacuum fluctuations.1 The structure used was a colloidal crystal with a face-centered cubic structure whose (111) planes were separated by optical dimensions.
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.
We observed for the first time a strong angle-independent modification of spontaneous emission spectra from laser dyes in photonic crystals, made of inverse opals in titania. Comparison with spectra from such crystals with much smaller lattice spacing, for which emission is in the long wavelength limit, reveals inhibition of emission up to a factor approximately 5 over a large bandwidth of 13% of the first order Bragg resonance frequency. The center frequency and bandwidth of the inhibition agree with calculated total density of states, while the measured inhibition of vacuum fluctuations is much larger. Because of the specific location of the dye molecules, we likely probe the strongly modulated local photonic density of states.
We have measured the radiative transition rate of Eu3+{\mathrm{Eu}}^{3+}Eu3+ complexes in polystyrene films on various dielectric substrates. Both inhibition and enhancement of the transition rate are observed, depending on the refractive index of the substrate and thickness of the film. This is explained in terms of local photon mode amplitudes.