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Physical Review A

Spontaneous emission in absorbing dielectrics: A microscopic approach

Gediminas Juzeliūnas, A. Gos, W Xa

Published Jan 1, 1997• 4 citations
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Abstract

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.

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Spontaneous emission in absorbing dielectric media

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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.

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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.
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.
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 lifetime of an excited atom near an absorbing dielectric surface is calculated from an exact solution of a microscopic Hamiltonian model, which includes the effects of dispersion, local-field correction, and near-field Coulomb interaction. Results for the total decay rate are shown to be in excellent agreement with those based on classical electromagnetic theory and to yield the well-known result for the rate of nonradiative energy transfer in the limit of very small distance from the surface. \textcopyright{} 1996 The American Physical Society.
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 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.
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.