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Physical Review A

Microscopic theory of quantization of radiation in molecular dielectrics. II. Analysis of microscopic field operators

Gediminas Juzeliūnas

Published Feb 1, 1997• 16 citations
Publisher

Abstract

The microscopic operators have been investigated for radiation and polarization fields within a discrete molecular medium. The medium comprises atoms (or molecules) each containing an arbitrary number of energy levels. Explicit mode expansions have been derived for the quantized microfields in terms of normal Bose operators for polariton creation and annihilation. These microscopic operators have been demonstrated to yield the correct macroscopic and local field operators presented in part I [Phys. Rev. A 53, 3543 (1996)]. On the other hand, the commutation relations between the expanded microfields differ from the exact commutation relationships. This happens because the microfields have been described in terms of a continuous refractive index. Hence the expanded field operators do not extend to modes with extremely high frequencies ranging over the photon umklapp frequencies cG. In spite of that, the proper commutation relations hold between the resultant macroscopic (averaged) fields. This justifies separate quantization of the slowly modulated (macroscopic) part of the radiation field in linear dielectrics: such an approach is utilized in phenomenological quantization schemes. Finally, although the microscopic operators presented are not complete, the mode expansions adequately represent the quantized microfields associated with the optical modes in condensed molecular media.

DOI
10.1103/physreva.55.929

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The microscopic operators have been investigated for radiation and polarization fields within a discrete molecular medium. The medium comprises atoms (or molecules) each containing an arbitrary number of energy levels. Explicit mode expansions have been derived for the quantized microfields in terms of normal Bose operators for polariton creation and annihilation. These microscopic operators have been demonstrated to yield the correct macroscopic and local field operators presented in part I [Phys. Rev. A 53, 3543 (1996)]. On the other hand, the commutation relations between the expanded microfields differ from the exact commutation relationships. This happens because the microfields have been described in terms of a continuous refractive index. Hence the expanded field operators do not extend to modes with extremely high frequencies ranging over the photon umklapp frequencies cG. In spite of that, the proper commutation relations hold between the resultant macroscopic (averaged) fields. This justifies separate quantization of the slowly modulated (macroscopic) part of the radiation field in linear dielectrics: such an approach is utilized in phenomenological quantization schemes. Finally, although the microscopic operators presented are not complete, the mode expansions adequately represent the quantized microfields associated with the optical modes in condensed molecular media.
Theories which have been used to describe the quantized electromagnetic field interacting with a nonlinear dielectric medium are either phenomenological or derived by quantizing the macroscopic Maxwell equations. Here we take a different approach and derive a Hamiltonian describing interacting fields from one which contains both field and matter degrees of freedom. The medium is modeled as a collection of two-level atoms, and these interact with the electromagnetic field. The atoms are grouped into effective spins and the the Holstein-Primakoff representation of the spin operators is used to expand them in inverse powers of the total spin. When the lowest order term of the interaction is combined with the free atomic and field Hamiltonians, a Hamiltonian describing a theory of noninteracting polaritons results. When higher order terms are expressed in terms of polariton operators standard nonlinear optical interactions emerge. These are then compared to the results of phenomenological and macroscopic theories. The theory is also used to derive an effective Hamiltonian describing counterpropagating modes in a nonlinear medium.
We present a fully canonical quantization scheme for the electromagnetic field in dispersive and lossy linear dielectrics. This scheme is based on a microscopic model, in which the medium is represented by a collection of interacting matter fields. We calculate the exact eigenoperators for the coupled system and express the electromagnetic field operators in terms of them. The dielectric constant of the medium is explicitly derived and is shown to satisfy the Kramers-Kronig relations. We apply these results to treat the propagation of light in dielectrics and obtain simple expressions for the electromagnetic field in the medium in terms of space-dependent creation and annihilation operators. These operators satisfy a set of equal-space commutation relations and obey spatial Langevin equations of evolution. This justifies the use of such operators in phenomenological models in quantum optics. We also obtain two interesting relationships between the group and the phase velocity in dielectrics.
We derive the macroscopic electromagnetic-field and medium operators for a linear dispersive medium with a microscopic model. As an alternative to the previous treatments in the literature, we show that the canonical momentum for the macroscopic field can be chosen to be −∊0Ê instead of −Dˆ with the standard minimal-coupling Hamiltonian. We find that, despite the change in the field operator normalization constants, the equal-time commutators among the macroscopic electric-field, magnetic-field, and medium operators have the same values as their microscopic counterparts under a coarse-grained approximation. This preservation of the equal-time commutator is important from a fundamental standpoint, such as the preservation of micro-causality for macroscopic quantities. The existence of more than one normal frequency mode at each k vector in a realistic causal-response medium is shown to be responsible for the commutator preservation. The process of macroscopic averaging is discussed in our derivation. The macroscopic field operators we derive are valid for a wide range of frequencies below, above, and around resonances. Our derivation covers the lossless, slightly lossy, and dispersionless as well as dispersive regimes of the medium. The local-field correction is also included in the formalism by inclusion of dipole–dipole interactions. Comparisons are made with other derivations of the macroscopic field operators. Using our theory, we discuss the questions of field propagation across a dielectric boundary and the decay rate of an atom embedded in a dielectric medium. We also discuss the question of squeezing in a linear dielectric medium and the extension of our theory to the case of a nonuniform medium.
Macroscopic canonical quantization of the EM field and radiative atom systems occurring in quantum optics experiments involving linear classical optics devices can be carried out via expansion of the vector potential either in terms of true mode functions for the optical device or in terms of approximate or quasi mode functions. The relationship between the true mode and quasi mode annihilation, creation operators is determined and shown to involve a Bogolubov transformation. Analytic properties are also examined and it is found that the annihilation, creation operators times the square root of the angular frequency are analytic functions of the variables specifying the modes.
Recently Drummond and Hillery [Phys. Rev.A 59, 691(1999)] presented a quantum theory of dispersion based on the analysis of a coupled system of the electromagnetic field and atoms in the multipolar QED formulation. The theory has led to the explicit mode-expansions for various field-operators in a homogeneous medium characterized by an arbitrary number of resonant transitions with different frequencies. In this Comment, we drawn attention to a similar multipolar study by Juzeliunas [Phys. Rev.A 53, 3543 (1996); 55, 929 (1997)] on the field quantization in a discrete molecular (or atomic) medium. A comparative analysis of the two approaches is carried out, highlighting both common and distinctive features.
The problem of field quantization in a half space is discussed based on the detector modes, which provide a useful basis for the study of atomic or molecular interaction with radiation modes involving evanescent electromagnetic waves. The detector modes, each of which involves a single outgoing wave, are introduced in terms of the time-reversal and spatial-rotation transforms of the widely used triplet modes given by Carniglia and Mandel. The derivation of the orthogonal relation for the detector modes is therefore straightforward. We represent the creation and annihilation operators for the detector modes in terms of those for the triplet modes, and obtain the field operator, Hamiltonian, number operator, and pseudomomentum operator. Based on this formalism, we evaluate the differential radiation probability for atomic dipole radiation near a dielectric surface. The evaluation of the final-state mode density is straightforward for the detector modes involving single outgoing waves. With respect to the image dipole picture, the quantum-to-classical correspondence is clear in the detector-mode formalism.