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arXiv:quant-ph/9902076 · Physical Review A

Spontaneous emission and level shifts in absorbing disordered dielectrics and dense atomic gases: A Green’s-function approach

Michael Fleischhauer

Published Sep 1, 1999• 44 citations
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Abstract

Spontaneous emission and Lamb shift of atoms in absorbing dielectrics and dense atomic gases are discussed using a microscopic Green's-function approach. Uncorrelated and random atomic positions are assumed, and the associated unphysical interactions between different atoms at the same location are eliminated (local field correction). For the case of an atom in a purely dispersive medium, the spontaneous-emission rate is altered by the well-known Lorentz local-field factor. When the mean distance between atoms becomes less than the resonance wavelength, results different from previously suggested expressions are found. In particular, it is shown that nearest-neighbor interactions become important. The results suggest that, for large densities, absorbing disordered dielectrics cannot accurately be described by a macroscopic approach that neglects correlations between atomic positions.

DOI
10.1103/physreva.60.2534

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Spontaneous emission and Lamb shift of atoms in absorbing dielectrics and dense atomic gases are discussed using a microscopic Green's-function approach. Uncorrelated and random atomic positions are assumed, and the associated unphysical interactions between different atoms at the same location are eliminated (local field correction). For the case of an atom in a purely dispersive medium, the spontaneous-emission rate is altered by the well-known Lorentz local-field factor. When the mean distance between atoms becomes less than the resonance wavelength, results different from previously suggested expressions are found. In particular, it is shown that nearest-neighbor interactions become important. The results suggest that, for large densities, absorbing disordered dielectrics cannot accurately be described by a macroscopic approach that neglects correlations between atomic positions.
We have calculated the effect of material absorption on the rate of spontaneous emission by an embedded atom using a macroscopic Green-function approach and a microscopic Hamiltonian method that includes reservoir damping. When local field effects are neglected, the free-space emission rate is modified by the real part of the refractive index at the transition frequency of the embedded atom. Local field effects are introduced via a local field correction factor. This modification of the spontaneous emission rate generalizes a well-known result for transparent media and is of crucial importance in assessing the degree of inhibition of spontaneous emission for frequencies close to the resonances of the dielectric.
Local field effects on the rate of spontaneous emission and Lamb shift in a dense gas of atoms are discussed taking into account correlations of atomic center-of-mass coordinates. For this the exact retarded propagator in the medium is calculated in independent scattering approximation and employing a virtual-cavity model. The resulting changes of the atomic polarizability lead to modifications of the medium response which can be of the same order of magnitude but of opposite sign than those due to local field corrections of the dielectric function derived by Morice, Castin, and Dalibard [Phys.Rev.A 51, 3896 (1995)].
Resonant classical light scattering by impurity atoms inside dielectric cubic lattices is investigated in the point-dipole limit. Modifications to resonance frequencies and linewidths are shown to be different for substitutional and interstitial impurities. Spontaneous emission rates inside dielectrics exhibit the well-known empty-cavity and Lorentz local-field factors for substitutional and interstitial atoms, respectively. The results are generalized to disordered dielectrics, indicating that the substitutional case occurs prevalently for impurity atoms.
We consider the spontaneous emission in an absorbing medium by calculating the quantum flow of energy from an emitting atom. For this purpose, we extend the analysis by Power and Thirunamachandran of quantized Maxwell fields in the vicinity of an atom in the free space to a situation where the emitter is in a dielectric medium. We represent the quantum flow in terms of the non-equal time commutators involving electric and magnetic fields, as well as the local displacement field. The commutators are calculated applying a previously developed microscopic theory of quantization of radiation in dielectrics. Consequently, we derive from first principles the rate of spontaneous emission in an absorbing medium containing local field factors and other refractive contributions. The results support the previous introduction of the (virtual cavity) local field correction by Barnett et al on a phenomenological basis, as well as our previous approach in which the spontaneous emission is considered as a resonance energy transfer to the far-zone atoms. A distinctive feature of the present formalism is that it deals with the spontaneous emission directly by calculating the quantum flow from the emitting atom. Therefore, the method is free from divergences appearing in other approaches analysing the spontaneous decay in absorbing media.
Decay of an excited molecule (atom) has been considered in an absorbing dielectric. The decay rate has been derived calculating the total rate of excitation transfer to the surrounding species. The contribution due to the far-zone energy transfer yields the rate of photon emission in the absorbing medium. The analysis is based on a microscopic QED theory of energy transfer in condensed phases. As a result, effects due to discreteness of the medium (such as the local field effects) are reflected intrinsically in the decay rates. The microscopic approach supports the previous introduction of the local field factors on a phenomenological basis.
A formalism for studying spontaneous decay of an excited two-level atom in the presence of dispersing and absorbing dielectric bodies is developed. An integral equation, which is suitable for numerical solution, is derived for the atomic upper-state-probability amplitude. The emission pattern and the power spectrum of the emitted light are expressed in terms of the Green tensor of the dielectric-matter formation, including absorption and dispersion. The theory is applied to the spontaneous decay of an excited atom at the center of a three-layered spherical cavity, with the cavity wall being modeled by a band-gap dielectric of Lorentz type. Both weak and strong coupling are studied, the latter with a special emphasis on cases where the atomic transition is (i) in the normal-dispersion zone near the medium resonance, and (ii) in the anomalous-dispersion zone associated with the band gap. In a single-resonance approximation, conditions of the appearance of Rabi oscillations and closed solutions to the evolution of the atomic state population are derived, which are in good agreement with the exact numerical results.