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arXiv:quant-ph/0009057 · Physical Review A

Local-field corrections to the decay rate of excited molecules in absorbing cavities: The Onsager model

M. S. Tomaš

Published Apr 18, 2001• 45 citations
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Abstract

The decay rate and the classical radiation power of an excited molecule (atom) in the center of a dispersive and absorbing dielectric sphere, taken as a simple model of a cavity, are calculated adopting the Onsager model for the local field. The local-field correction factor to the external (radiation and absorption) power loss of the molecule is found to be $|3\ensuremath{\varepsilon}(\ensuremath{\omega})/[3\ensuremath{\varepsilon}(\ensuremath{\omega})+1]{|}^{2},$ with $\ensuremath{\varepsilon}(\ensuremath{\omega})$ being the dielectric function of the sphere. However, local-field corrections to the total decay rate (power loss) of the molecule are found to be much more complex including those to the decay rate in the infinite cavity medium, as derived recently by Scheel et al. [Phys. Rev. A $60,$ 4094 (1999)], and similiar corrections to the cavity-induced decay rate. The results obtained can be cast into general forms that do not rely on the specific cavity shape and molecule position considered. This suggests the general results for the local-field corrections to the decay rate and to the external power loss of a molecule in an absorbing cavity that are valid for molecule positions away from the cavity walls.

DOI
10.1103/physreva.63.053811

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The decay rate and the classical radiation power of an excited molecule (atom) in the center of a dispersive and absorbing dielectric sphere, taken as a simple model of a cavity, are calculated adopting the Onsager model for the local field. The local-field correction factor to the external (radiation and absorption) power loss of the molecule is found to be ∣3\ensuremathε(\ensuremathω)/[3\ensuremathε(\ensuremathω)+1]∣2,|3\ensuremath{\varepsilon}(\ensuremath{\omega})/[3\ensuremath{\varepsilon}(\ensuremath{\omega})+1]{|}^{2},∣3\ensuremathε(\ensuremathω)/[3\ensuremathε(\ensuremathω)+1]∣2, with \ensuremathε(\ensuremathω)\ensuremath{\varepsilon}(\ensuremath{\omega})\ensuremathε(\ensuremathω) being the dielectric function of the sphere. However, local-field corrections to the total decay rate (power loss) of the molecule are found to be much more complex including those to the decay rate in the infinite cavity medium, as derived recently by Scheel et al. [Phys. Rev. A 60,60,60, 4094 (1999)], and similiar corrections to the cavity-induced decay rate. The results obtained can be cast into general forms that do not rely on the specific cavity shape and molecule position considered. This suggests the general results for the local-field corrections to the decay rate and to the external power loss of a molecule in an absorbing cavity that are valid for molecule positions away from the cavity walls.
The decay rate of an excited molecule (atom) embedded in a dispersive and absorbing planar cavity is derived by using a recently obtained compact form of the Green's function for a multilayer. As a by-product, a hint is provided for a straightforward extension of the results obtained for lossless cavities of other shapes to the corresponding absorbing cavities. The decay rate in an absorbing cavity consists of the spontaneous emission rate and of the nonradiative rates caused by the near-field interaction of the molecule with the cavity medium and, for nearby molecules, with the cavity mirrors. Only the spontaneous emission rate is satisfactorily described in the macroscopic approach adopted. The theory is applied to an analysis of the effects of the weak cavity absorption on the decay rate in a dielectric microcavity formed by two metallic mirrors. As expected, dissipation in the cavity medium spoils the conditions for controlled spontaneuos emission and strongly suppresses the intensity of spontaneous emission. However, its effect on the spontaneous emission rate is much less pronounced.
A recently developed scheme [S. Scheel, L. Kn\"oll, and D.-G. Welsch, Phys. Rev. A 58, 700 (1998)] for quantizing the macroscopic electromagnetic field in linear dispersive and absorbing dielectrics satisfying the Kramers-Kronig relations is used to derive the quantum local-field correction for the standard virtual-sphere-cavity model. The electric and magnetic local-field operators are shown to become approximately consistent with QED only if the polarization noise is fully taken into account. It is shown that the polarization fluctuations in the local field can dramatically change the spontaneous decay rate, compared with the familiar result obtained from the classical local-field correction. In particular, the spontaneous emission rate strongly depends on the radius of the local-field virtual cavity.
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.
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 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.