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Physical Review Letters

Suppression of Molecular Interactions in Periodic Dielectric Structures

Gershon Kurizki, Azriel Z. Genack

Published Nov 7, 1988• 112 citations
Publisher

Abstract

We show that resonant dipole-dipole interactions are suppressed at all interatomic or intermolecular separations in periodic dielectric structures in which spontaneous emission is inhibited at the resonant optical transitions. This profoundly modifies molecular properties including donor-acceptor energy transfer, collisional dynamics, molecular spectra, and dissociation energies.

DOI
10.1103/physrevlett.61.2269

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We show that resonant dipole-dipole interactions are suppressed at all interatomic or intermolecular separations in periodic dielectric structures in which spontaneous emission is inhibited at the resonant optical transitions. This profoundly modifies molecular properties including donor-acceptor energy transfer, collisional dynamics, molecular spectra, and dissociation energies.
Radiative coupling between identical atoms sharing an excitation is studied in media where dispersion creates photonic band gaps, i.e., forbidden bands of light propagation for all directions and polarizations. Photonic band gaps can exist in media whose dielectric index exhibits strong three-dimensionally periodic modulations (``photonic crystals'') or in bands of polaritonic media. It is shown that the resonant dipole-dipole interaction as well as cooperative fluorescence of two-atom systems can be strongly enhanced or suppressed, to the extent of being essentially eliminated, by one of the following mechanisms: (a) dependence on location of the atoms within a unit cell of a photonic crystal, i.e., sensitivity to the spatial variation of the field normal modes; (b) dependence on the density of normal modes in allowed bands and on the density of virtual (evanescent) modes in band gaps. The ability to suppress the dipole-dipole interactions at interatomic separations characterizing quasimolecules would have far-reaching implications on their dissociative or collisional dynamics, spectroscopy, and rates of energy transfer.
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 show rigorously that the coefficient for spontaneous emission of an atom placed in a dielectric is proportional to the local radiative density of states—that is only a part of the local density of the eigenmodes of the Maxwell equations. Spontaneous emission is inhibited if the atom is located at a position where this local radiative density is small, even if the total density of states is not vanishing. This radiative density of states can be obtained without having to perform a full quantum calculation of the radiation-matter system. We demonstrate this principle by solving numerically a scalar model for a dielectric that consists of a lattice of resonating dipoles.
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.