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Progress of Theoretical Physics Supplement

Nonlocal Theory of Radiation-Matter Interaction: Boundary-Condition-Less Treatment of Maxwell Equations

Kikuo Cho

Published Jan 1, 1991• 104 citations
Publisher

Abstract

Based on the separability with respect to position variables of the susceptibility for a finite system, we have developed a formulation which solves Schri:idinger and Maxwell equations selfconsistently. The case of linear response is' described in detail. As a manifes­ tation of the selfconsistency between the two equations, the appearance of radiative damping rate with correct magnitude has been demonstrated for a two-level atom in vacuum. The interaction of electromagnetic (EM) radiation with matter has been studied in various aspects for quite a long time. The relevant phenomena range, in the scale of wavelength, from rf wave (NMR, for example) to gamma ray (Mossbauer effect): They are related with the absorption, reflection, transmission, propagation, refrac­ tion, scattering, diffraction, emission, etc. of EM wave in linear and nonlinear manner. For the theoretical treatment of these phenomena, we need Schrodinger equation for the description of matter and Maxwell equations in classical or quantized form for radiation field. When the Maxwell equations are treated in classical form, this is called semiclassical treatment of radiation-matter interaction. Though it has a certain limitation, the semiclassical treatment can be appliedto most of the phenom­ ena mentioned above. For the treatment of the interaction of EM radiation with solids, it is usual to employ a susceptibility function to describe the solid, and solve the Maxwell equa­ tions containing that susceptibility as an integral kernel. In doing so, we must consider the boundary conditions (BC) arising from the shape of the sample in question. However, we do not consider BC's in treating microscopic systems such as an atom or small molecule. This would mean that the use of BC(s is in general not compulsory, although we are so much accustomed to it. In this respect, there has been a long debated problem of additional boundary condition (ABC) in relation with exciton polaritons in semiconductors or insulators, where the nonlocal nature of the medium allows the existence of two or more eigenmodes of the coupled exciton-EM radiation. After the long history of the ABC problem,r>- 4 > we now have a recipe to derive the appropriate form(s) of ABC(s) from a microscopic model of the medium including the details of the surface. 5 >-s> Another form of the microscopic solution of the ABC problem has been given as an ABC-free formulation, 9 >-n> where one needs

DOI
10.1143/ptps.106.225

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Nonlocal Theory of Radiation-Matter Interaction: Boundary-Condition-Less Treatment of Maxwell Equations

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Based on the separability with respect to position variables of the susceptibility for a finite system, we have developed a formulation which solves Schri:idinger and Maxwell equations selfconsistently.The case of linear response is' described in detail.As a manifestation of the selfconsistency between the two equations, the appearance of radiative damping rate with correct magnitude has been demonstrated for a two-level atom in vacuum.§ 1. Introduction

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Based on the separability with respect to position variables of the susceptibility for a finite system, we have developed a formulation which solves Schri:idinger and Maxwell equations selfconsistently. The case of linear response is' described in detail. As a manifes­ tation of the selfconsistency between the two equations, the appearance of radiative damping rate with correct magnitude has been demonstrated for a two-level atom in vacuum. The interaction of electromagnetic (EM) radiation with matter has been studied in various aspects for quite a long time. The relevant phenomena range, in the scale of wavelength, from rf wave (NMR, for example) to gamma ray (Mossbauer effect): They are related with the absorption, reflection, transmission, propagation, refrac­ tion, scattering, diffraction, emission, etc. of EM wave in linear and nonlinear manner. For the theoretical treatment of these phenomena, we need Schrodinger equation for the description of matter and Maxwell equations in classical or quantized form for radiation field. When the Maxwell equations are treated in classical form, this is called semiclassical treatment of radiation-matter interaction. Though it has a certain limitation, the semiclassical treatment can be appliedto most of the phenom­ ena mentioned above. For the treatment of the interaction of EM radiation with solids, it is usual to employ a susceptibility function to describe the solid, and solve the Maxwell equa­ tions containing that susceptibility as an integral kernel. In doing so, we must consider the boundary conditions (BC) arising from the shape of the sample in question. However, we do not consider BC's in treating microscopic systems such as an atom or small molecule. This would mean that the use of BC(s is in general not compulsory, although we are so much accustomed to it. In this respect, there has been a long debated problem of additional boundary condition (ABC) in relation with exciton polaritons in semiconductors or insulators, where the nonlocal nature of the medium allows the existence of two or more eigenmodes of the coupled exciton-EM radiation. After the long history of the ABC problem,r>- 4 > we now have a recipe to derive the appropriate form(s) of ABC(s) from a microscopic model of the medium including the details of the surface. 5 >-s> Another form of the microscopic solution of the ABC problem has been given as an ABC-free formulation, 9 >-n> where one needs
Annalen der Physik , Ser. 5, 9: 338–46 (1931). Received 25 February 1931. The Dirac theory of radiation gives a satisfactory account of the absorption, emission, and dispersion of radiation by atoms. Beyond this, quantum electrodynamics also provides a satisfactory treatment of interference phenomena. The results of the theory in most cases agree with what is expected from the correspondence principle, but the calculations which lead to this objective have hitherto been rather complicated, and the simplest consequences of classical radiation theory can only be derived along the circuitous route through a quite nontransparent Schrödinger equation in an infinite-dimensional space. Below we shall describe a method for treating radiation problems which connects, much more closely than the previous ones, the intuitive conceptions of classical theory with those of wave mechanics and which therefore, in most cases, and without detours, yields the result expected in terms of the correspondence principle. In this method, the starting point shall not be the Hamiltonian function or the corresponding Schrödinger equation in configuration space but rather the equations of motion, i.e. the Maxwell and Dirac wave equations. These differential equations are integrated explicitly, after the value of the wave functions ( E, H , and ψ σ ) at time t = 0 are regarded as given; here it should be noted that the wave functions at time t = 0 are noncommuting quantities. This noncommutability of the initial values of E, H , and ψ σ does not disturb the integration, however, as long as the interaction between matter and radiation is assumed to be small and only linear terms in this interaction are considered.
We investigate in this chapter the general problem of the interaction of an atom (or a molecule) and a classical electromagnetic field. Its importance derives firstly from the fact that a large part of our knowledge of atoms is obtained from a study of the radiation they absorb or emit (we shall consider equally visible radiation and radio-frequency and X-rays) and, secondly, that the interaction with matter modifies the propagation of the electromagnetic field itself, notably through absorption, refraction or scattering. The interactions of atoms with light therefore encompass a vast range of physical effects that we could not hope to cover adequately in a single chapter. In this chapter we shall therefore present the fundamental features of the interaction of an atom, which will be treated quantum mechanically, with a classical electromagnetic field, that is an electromagnetic field described by real electric and magnetic vectors obeying Maxwell's equations. A rigorous description of the atom–light interaction would have to take into account the quantum nature of light. This we shall leave to Chapter 6. It turns out, nevertheless, that many important results can be obtained from the semi-classical viewpoint adopted here (although it is perhaps more appropriate to refer to this treatment as ‘semi-quantized’).
A rigorous description of the light–matter interaction requires the use of quantized Maxwell equations to describe the light field and the Schrödinger equation to describe the material medium. This book does not attempt to deal with quantum optical problems that necessitate a field quantization. Instead we focus on properties that are generally grouped under the umbrella of nonlinear optics . Although many definitions of this expression exist, we use it in the sense that the properties we deal with do not depend in a crucial way on the field quantization. For practical purposes, this means in general that the average photon number is large and that we can neglect spontaneous emission as a dynamical process. Rather, we include the consequence of spontaneous emission, that is, the instability of the atomic levels, in a purely phenomenological way. When this is done, we call the material equations the Bloch equations instead of the Schrödinger equation. References [1] through [4] are the classical textbooks that contain a tentative justification for the transition from the Schrödinger to the Bloch equations. None of these attempts is satisfactory from a fundamental viewpoint because the real difficulty is to incorporate the finite lifetime (or natural linewidth) of the atomic energy levels in the Schrödinger equation. This remains an open problem as of now. The Maxwell–Schrödinger equations We consider atoms interacting with an intense electromagnetic field. By intense we mean a field for which the quantization is not necessary.
This chapter considers an atom as a quantum mechanical system. But the electromagnetic radiation will be treated as classical waves described by the Maxwell equations. The treatment is called semi-classical. Quantum mechanics describes an atom as a quantized system with a set of discrete energy levels. Each energy level is designated by a set of quantum numbers like the principal quantum of the Rydberg level and the quantum numbers representing the orbital, spin and total angular momentum. A molecule will have a different set of quantum numbers arising from its rotational and vibrational motions. Atoms in a solid have energy levels in the form of a band. The observed spectrum due to spontaneous emission from a collection of atoms is not monochromatic, but it is spread over a certain range of frequencies. The absorption spectrum also shows that the atom does not absorb at a single frequency, but it is spread over a band of frequencies around the resonance frequency.
Classical, semi-classical, and quantum-field descriptions for the interaction of light with matter are systematically discussed. Applications of interest include precise determinations of the linear and the non-linear electromagnetic response relevant to resonant pump-probe optical phenomena, such as electromagnetically induced transparency. In the quantum-mechanical description of matter systems, we introduce a general reduced-density-matrix framework. Time-domain (equation-of-motion) and frequency-domain (resolvent-operator) formulations are developed in a unified and self-consistent manner, using a Liouville-space operator representation. A preliminary semi-classical perturbation treatment of the electromagnetic interaction is adopted, in which the electromagnetic field is described as a classical field satisfying the Maxwell equations. Compact Liouville-space operator expressions are derived for the linear and the general (nth order) non-linear electromagnetic-response tensors describing moving many-electron systems. The tetradic matrix elements of the Liouville-space self-energy operators, which are introduced in the time-domain and frequency-domain formulations, are evaluated for environmental collisional and radiative interactions, in order to provide explicit forms for the quantum kinetic equations and the spectral-line shape formulas. It is emphasized that a quantized-field approach is essential for a fully self-consistent quantum-mechanical description of the interacting light-matter system.