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Journal of Physics B Atomic Molecular and Optical Physics

Decay of excited atoms in absorbing dielectrics

Stephen Mark Barnett, B. Hüttner, R. Loudon, Reza Matloob

Published Aug 28, 1996• 177 citations
Publisher

Abstract

We present calculations of the rates of decay of an excited atom embedded in an absorbing dielectric. Decay can occur by spontaneous emission into transverse radiative modes of the electromagnetic field and by Joule heating via longitudinal coupling of the atom to the dielectric. The spontaneous emission (transverse) decay rate is modified in a dielectric, being the free-space rate multiplied by the real part of the refractive index at the transition frequency of the atom. There is a further modification due to the difference between the macroscopic dielectric field and the local field at the position of the atom. In addition there is a longitudinal decay rate which is proportional to the imaginary part of the dielectric constant and therefore vanishes in non-absorbing media. We derive expressions for each of these rates of decay and discuss the physical mechanisms leading to them.

DOI
10.1088/0953-4075/29/16/019

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We present calculations of the rates of decay of an excited atom embedded in an absorbing dielectric. Decay can occur by spontaneous emission into transverse radiative modes of the electromagnetic field and by Joule heating via longitudinal coupling of the atom to the dielectric. The spontaneous emission (transverse) decay rate is modified in a dielectric, being the free-space rate multiplied by the real part of the refractive index at the transition frequency of the atom. There is a further modification due to the difference between the macroscopic dielectric field and the local field at the position of the atom. In addition there is a longitudinal decay rate which is proportional to the imaginary part of the dielectric constant and therefore vanishes in non-absorbing media. We derive expressions for each of these rates of decay and discuss the physical mechanisms leading to them.
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.
Starting from the quantized version of Maxwell's equations for the electromagnetic field in an arbitrary linear Kramers-Kronig dielectric, the Heisenberg equations of motion for a two-level atom resonantly coupled to the radiation field in the presence of dispersive and absorbing dielectric bodies are derived. The theory is applied to the problem of spontaneous decay of excited atoms in absorbing media. The decay rate is calculated for the (Glauber-Lewenstein) real-cavity model, and a comparison with the recently studied (Clausius-Mosotti) virtual-cavity model [S. Scheel, L. Kn\"oll, D.-G. Welsch, and S. M. Barnett, Phys. Rev. A 60, 1590 (1999)] is given. It is shown that owing to nonradiative decay associated with absorption, the rate of spontaneous decay sensitively depends on the cavity radius, particularly when the atomic transition frequency approaches an absorption band of the medium. Only when the effect of absorption is fully disregarded, is the familiar local-field correction factor recovered.
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.
The spontaneous-emission rate of a radiating atom reaches its time-independent equilibrium value after an initial transient regime. In this paper, we consider the associated relaxation effects of the spontaneous-decay rate of atoms in dispersive and absorbing dielectric media for atomic-transition frequencies near material resonances. A quantum mechanical description of such media is furnished by a damped-polariton model in which absorption is taken into account through coupling to a bath. We show how all field and matter operators in this theory can be expressed in terms of the bath operators at an initial time. The consistency of these solutions for the field and matter operators are found to depend on the validity of certain velocity sum rules. The transient effects in the spontaneous-decay rate are studied with the help of several specific models for the dielectric constant, which are shown to follow from the general theory by adopting particular forms of the bath coupling constant.
We have computed the spontaneous decay rate of an atom placed inside an absorbing dielectric adopting the real cavity model. The calculations are performed applying a quantization scheme which is causal and fully consistent with the dissipation-fluctuation theorem. We have started with a full electric field operator and found that the decay rate contains only contributions from the transverse field and sensitively depends on the cavity radius - results that contradict earlier results derived on the basis of heuristic introduction of local-field correction factors.