Classical dispersion theory Many aspects of the interaction between radiation and matter can be described quite accurately by a classical theory in which the medium is represented by model atoms consisting of positive and negative parts bound by an attraction which depends linearly on their separation. Although quantum theory is necessary to calculate from first principles the magnitude of the parameters involved, in this chapter we shall show that many optical effects can be interpreted physically in terms of this model by the use of classical mechanics. In §13.5 we shall relax the restriction of linearity. Some of the quantum mechanical foundations will be discussed briefly in Chapter 14, but most are outside the scope of this book (see Yariv, 1989; Loudon, 1983). The term dispersion means the dependence of dielectric response (dielectric constant and refractive index) on frequency of the wave field. This will be the topic of the present section. Afterwards we shall see some of the applications of dielectric response to spatial effects. The classical atom Our classical picture of an atom consists of a massive positive nucleus surrounded by a light spherically-symmetrical cloud of electrons with an equal negative charge. We imagine the two as bound together by springs as in Fig. 13.1, so that in equilibrium the centres of mass and charge of the core and electron charge coincide. As a result the static atom has zero dipole moment.
Classical dispersion theory Many aspects of the interaction between radiation and matter can be described quite accurately by a classical theory in which the medium is represented by model atoms consisting of positive and negative parts bound by an attraction which depends linearly on their separation. Although quantum theory is necessary to calculate from first principles the magnitude of the parameters involved, in this chapter we shall show that many optical effects can be interpreted physically in terms of this model by the use of classical mechanics. In §13.5 we shall relax the restriction of linearity. Some of the quantum mechanical foundations will be discussed briefly in Chapter 14, but most are outside the scope of this book (see Yariv, 1989; Loudon, 1983). The term dispersion means the dependence of dielectric response (dielectric constant and refractive index) on frequency of the wave field. This will be the topic of the present section. Afterwards we shall see some of the applications of dielectric response to spatial effects. The classical atom Our classical picture of an atom consists of a massive positive nucleus surrounded by a light spherically-symmetrical cloud of electrons with an equal negative charge. We imagine the two as bound together by springs as in Fig. 13.1, so that in equilibrium the centres of mass and charge of the core and electron charge coincide. As a result the static atom has zero dipole moment.
The classical theory of the interaction of light with the electron clouds of atoms and molecules will be discussed in this chapter. The discussion will begin with the interaction of a steady electric field with a collection of point charges, leading to the development of terms describing the electric dipole and quadrupole moments. The classical Lorentz model is then introduced to describe interaction of an oscillating electric field with the electron cloud of an atom, and the concepts of absorption and emission are introduced. The propagation of a light wave through a medium with electric dipoles is then discussed. Finally, the classical theory of radiation from an oscillating dipole is discussed.
This first complement is devoted to a completely classical approach of lightmatter interaction which was proposed by Lorentz at the end of the nineteenth century, before the advent of quantum mechanics, but after the discovery of the electron. Lorentz' phenomenological model is based on the experimental fact that atoms have well-defined and sharp absorption lines: he assumed that atoms behaved like harmonic oscillators, in which the electrons are bound to the atomic nucleus by a restoring force which varies linearly with its displacement (from its equilibrium point close to a nucleus), and makes them oscillate at a given frequency ω 0 equal to the experimentally determined absorption frequency. Within the frame of this model, we first calculate the electromagnetic field radiated by an oscillating electron. We show that in the absence of an externally applied force the free oscillations of the electron are damped, because electromagnetic energy is radiated at the expense of mechanical energy. We then study the characteristics of the radiation that is emitted when the oscillations are forced by the application of an external oscillatory electromagnetic field of angular frequency ω. We characterize the different regimes of this scattering of the incident electromagnetic wave and finally determine the polarization induced in the atomic medium by the incident electromagnetic wave. The Lorentz model can be considered as a lowest order approximation to a description of the light–matter interaction, a better approximation being the semi-classical treatment presented in Chapter 2, and the rigorous treatment being the completely quantum mechanical model presented in Chapter 6.
Thus far, we have developed the properties of the electromagnetic field at optical frequencies, based on Maxwell’s equations. These equations further give a classical macroscopic perspective on the coupling of the propagation media to the field, as presented in Chapter 2. The macroscopic properties of a medium are based on averaged microscopic properties. The microscopic energy structure of matter was presented in Chapter 3, covering gases, solids, and liquids by employing mostly quantum models. We now proceed to the next level of development, the dynamic description of the interaction between the optical field and the propagation medium as a function of the field frequency and propagation media variables (e.g., energy structure, temperature, and pressure). In this chapter, the classical electromagnetic field is coupled to discrete frequency oscillators via Newton’s equation of motion. This approach leads to the popular classical oscillator model, often presented in introductory books on lasers. The classical oscillator model is an incomplete theory and can be only a semiempirical model. In the next chapter, a more detailed and comprehensive approach, which also includes statistical and quantum mechanics, is used leading to robust semiclassical and quantum oscillator models. This chapter and the next are the basis for the applied models presented in Part II of this book. Classical electrodynamics is based on Maxwell’s equations, as given in Chapter 2, and the Lorentz force relation, as given below: . . . F = q[E + (v × B)]. (4.1) . . . These equations cover the classical description of the interaction of light and matter. The first term in Eq. 4.1 represents coupling of the electric field to the medium. As discussed in Chapter 2 (Section 2.2), the leading mechanism for this is the electric dipole moment. To see that this is the coupling mechanism in the first term, consider the potential function driving this force, F = −∇V(r) = −∇(−qr · E). The above expression contains the dipole moment, as defined in Chapter 2. The second term in Eq. 4.1 represents coupling of the magnetic field to the medium.
This chapter presents the electron oscillator model of light-matter interaction. It models atomic response to the fields in an electromagnetic wave after a classical driven charged (dipole) oscillator. It is used to calculate atomic polarization and dielectric susceptibility and derive an equation of motion for atomic polarization for a collection of atoms. By replacing the oscillator number density in this equation with the level population density difference and interpreting oscillator frequency with transition frequency and decay rate with spontaneous emission rate a quantum mechanically correct equation for atomic polarization is obtained. Poynting theorem on energy exchange between light and atoms in an EM wave then yields quantum mechanically correct rate equations for population densities. These equations together with the equation for atomic polarization provide a complete description of atomic response to light. Modifications to the atomic response due to finite atomic lifetimes, collisions, atomic motion, local variation of resonance frequency and other factors are also discussed in terms of lineshape function and cross-section.
Atoms and ions containing residual bound electrons do not quite resemble the simple harmonic oscillator model used so successfully in the classical theory of radiation. However, replacing the atoms or ions with sets of harmonic oscillators of a great number of discrete resonance frequencies and having various amplitudes, together with the results of classical radiation theory, go a long way toward a quantitative description of emission or absorption spectra. The set of resonance frequencies is obtained from measured or calculated energy levels using Ritz's combination principle. The amplitudes are associated with matrix elements of appropriate quantum mechanical operators between wave functions of the two energy eigenstates involved at a given frequency. In other words, quantities of the emitters, absorbers, or scatterers are described quantum-mechanically, whereas the electromagnetic field is treated classically. Such semi-classical description of matter-electromagnetic field interactions became unnecessary very early in the development of quantum theory. It will therefore not be discussed in any detail. Instead, we will begin immediately with the combined theory of matter and radiation (Heitler 1954, Dirac 1958, Loudon 1983). Quantum theory of particles and fields There are various ways to also quantize the electromagnetic fields (Cohen-Tannoudji, DuPont-Roc and Grynberg 1989), of which that performed on the combined Hamiltonian equations of motion for the field-matter system is followed here.
Although the primarily phenomenological theory of absorption and refraction of light by matter, based on classical models as presented in Chapter 4, is very useful, it is incomplete and often inadequate. A more complete and accurate picture of electrodynamics is given by the theory of quantum optics, and that is the topic of this chapter. The models developed in this chapter are more detailed and therefore more complicated than the phenomenological models of Chapter 4. The most robust models, which are applied in Part II, are presented in this chapter. The quantum models accurately represent experimental data and allow extrapolation and interpolation of such data. Many practical computer based models concerning optical propagation are based on this theory. The theory of elastic scatter as presented in Chapter 4 is consistent with quantum optics and is not presented again. (However, inelastic scatter must address the quantum nature of the scattering medium.) Quantum optics is not completely covered in this chapter. Entire textbooks are devoted to this diverse and comprehensive topic covering optics (see Refs. 5.1–5.3). The emphasis of this book is on absorption and reflection spectroscopy. Now details of internal structure of the medium impacting light–matter interaction are examined. The classical oscillator model is upgraded by semiclassical radiation theory and a quantum oscillator model is developed. Semiclassical radiation theory is based on a quantized medium coupled to a classical field. It is often applied to laser theory, where near-line-center stimulated emission dominates. The quantum oscillator model again utilizes the quantized medium and classical field, but with more attention to detailed balance between absorption and emission. It satisfies causality and the fundamental symmetry relationships established in Chapter 2. These quantum optics models are more complete formalisms and provide solutions to the shortcomings of classical electrodynamics. Of particular interest to propagation in gaseous media is the line shape in the far wing. To achieve long path lengths, propagation near line center of a resonance must be avoided. Line shape models in quantum optics accurately represent much of the frequency and temperature dependence observed in experimental data.