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Physical Review A

Lorentz local-field effects on spontaneous emission in dielectric media

Michael E. Crenshaw, Charles M. Bowden

Published Nov 29, 2000• 19 citations
Publisher

Abstract

The recent first-principles derivation of Langevin-Bloch equations of motion for near-resonant atoms embedded in a linear dielectric host leads to a clear, direct physical reinterpretation of fundamental physical principles as applied to one of the most basic problems of quantum mechanics: the renormalization of the spontaneous emission rate of an atom in a dielectric host. Here we show the role of the Lorentz local field, the fluctuation-dissipation theorem, the wave number and wave vector, the density of states, Fermi's golden rule, the electromagnetic energy density, canonical quantization, and the classical constitutive relations in this context.

DOI
10.1103/physreva.63.013801

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The recent first-principles derivation of Langevin-Bloch equations of motion for near-resonant atoms embedded in a linear dielectric host leads to a clear, direct physical reinterpretation of fundamental physical principles as applied to one of the most basic problems of quantum mechanics: the renormalization of the spontaneous emission rate of an atom in a dielectric host. Here we show the role of the Lorentz local field, the fluctuation-dissipation theorem, the wave number and wave vector, the density of states, Fermi's golden rule, the electromagnetic energy density, canonical quantization, and the classical constitutive relations in this context.
In this work the electromagnetic field in a dielectric medium is quantized in a simple and straightforward way based on the classical expression for the energy density for the case of weak absorption. The quantized field leads to expressions for spontaneous and stimulated emission rates, and gain and absorption coefficients, for the general case of a dispersive dielectric host medium. Local field corrections, when they apply, arise in the same manner as in classical electromagnetic theory. The theory also leads to a radiative level shift dependent on the dispersion of the dielectric, and this shift may be interpreted as a van der Waals interaction between the guest atom and the atoms of the host medium.>
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.
Summary form only given. The dynamics of a medium consisting of a dense collection of two-level atoms interacting via the electromagnetic field has been derived from first principles. In dense media and condensed matter, the microscopic local field that couples with a single atom is related to the macroscopic field and volume propagation by the Lorentz-Lorenz relation written for an isotropic homogeneous medium. The dynamical equations for the medium, coupled self-consistently with the Maxwell inhomogeneous wave equation, are given in the rotating wave and dipole coupling approximations. The microscopic development is used within the framework of full quantization, and the explicit effects of spontaneous relaxation for the host as well as the atoms are treated, together with corresponding fluctuations. Particular effects upon intrinsic adiabatic inversion, self-induced transparency, and lasing without inversion, are presented and discussed. In particular, the equilibrium, stationary, and dynamical effects of the host medium, and medium and field fluctuations upon local field effects are discussed.
The emission properties of atoms lie at the foundations of both quantum theory and light-matter interactions. In the context of macroscopic media, exact knowledge thereof is important both in current quantum technologies and in fundamental studies. While for isotropic media, this is a very well-studied problem, there are still big gaps in the theory of anisotropic media. In particular, to the best of our knowledge, an explicit expression for the spontaneous emission rate in general anisotropic media has not been presented. In this work, we first derive the quantized electromagnetic field operators to calculate the emission rate in uniaxial media. For the more general case of biaxial media we propose an approximate expression based on interpolation between the limiting cases of uniaxial media. We support our model with numerical simulations which are in strong agreement for typical media configurations and, furthermore, show how local field effects can be taken into account in the model.
The macroscopic quantum theory of the electromagnetic field in a dielectric medium interacting with a dense collection of embedded two-level atoms fails to reproduce a result that is obtained from an application of the classical Lorentz local-field condition. Specifically, macroscopic quantum electrodynamics predicts that the Lorentz redshift of the resonance frequency of the atoms will be enhanced by a factor of the refractive index nnn of the host medium. However, an enhancement factor of (n2+2)∕3({n}^{2}+2)∕3(n2+2)∕3 is derived using the Bloembergen procedure in which the classical Lorentz local-field condition is applied to the optical Bloch equations. Both derivations are short and uncomplicated and are based on well-established physical theories, yet lead to contradictory results. Microscopic quantum electrodynamics confirms the classical local-field-based results. Then the application of macroscopic quantum electrodynamic theory to embedded atoms is proved false by a specific example in which both the correspondence principle and microscopic theory of quantum electrodynamics are violated.