The classical theory of the interaction of radiation with matter developed by Einstein is part of the bag of tools of any scientist involved in radiation theory – the number of undergraduates who have been confused by ‘A’ and ‘B’ coefficients must be legion. Einstein's way of describing how photons are absorbed and emitted is so deeply ingrained in most scientists' understanding of radiation processes that they may forget that it is an approximate view of affairs. Classical broadband light sources – lamps – produce light whose influence on atoms can be described in terms of shunting populations between states. If one has a laser source, however, these simple pictures of population shunting may break down completely. It is essential when dealing with coherent sources to go back to the beginning and consider the dynamics of the radiation – matter interaction in detail.
The classical theory of the interaction of radiation with matter developed by Einstein is part of the bag of tools of any scientist involved in radiation theory – the number of undergraduates who have been confused by ‘A’ and ‘B’ coefficients must be legion. Einstein's way of describing how photons are absorbed and emitted is so deeply ingrained in most scientists' understanding of radiation processes that they may forget that it is an approximate view of affairs. Classical broadband light sources – lamps – produce light whose influence on atoms can be described in terms of shunting populations between states. If one has a laser source, however, these simple pictures of population shunting may break down completely. It is essential when dealing with coherent sources to go back to the beginning and consider the dynamics of the radiation – matter interaction in detail.
From prehistoric times has come recognition that sunlight and firelight provide warmth, and that such illumination casts shadows. Expressed in more contemporary terms one would say that light travels in rays, and that this radiation has the potential to provide heat energy to absorbing material. From the time of Newton it has been known that light sources emit radiation comprising a distribution of colors. During the nineteenth century it was recognized that radiation had characteristics of transverse waves (with wavelength associated to color) but until the late twentieth century, when lasers became laboratory tools, it was hardly necessary to delve into the equations of electromagnetic theory to treat such experiments as were then possible; interest lay primarily with thermodynamic considerations of energy flow or with measurements of the dark or bright lines seen in the distribution of light that, after passing through a slit, was dispersed by a prism or grating into constituent colors. Although laser light sources are essential for the types of atomic excitation considered in this monograph, the legacy from thermal radiation still influences many interpretations of the interaction between radiation and matter, and it is therefore useful to summarize some of those concepts. The mathematics needed for describing laser radiation, or polarized light in general, has much in common with the mathematics of quantum theory discussed starting in Sec. 3.5 and specialized to two-level atoms in Sec. 5.6. In both cases one deals with two complex-valued functions – independent electric field amplitudes or probability amplitudes – whose absolute squares are measurable.
The phenomena which are principally responsible for the interaction of radiation with matter in everyday life are absorption and spontaneous emis sion. Light falling on matter is absorbed, leaving atoms in excited states which spontaneously emit radiation with a spread of frequency inversely proportional to the decay time. The situation is modified when the atomic decay times are sufficiently long and the radiation sufficiently intense, for then radiation may fall on excited atoms, resulting in stimulated emission rather than absorption. We saw in Chap. 2 that this third process was required to obtain the Planck blackbody radiation law in Einstein’s derivation. It is stimulated emission which enables an atomic medium to amplify incident radiation, and therefore is an essential ingredient in light amplifiers and oscillators. In fact, the word LASER is an acronym for Light Amplification by Stimulated Emission of Radiation.
Many dynamical processes of interest are either initiated or probed by light, and their understanding requires some knowledge of this subject. This chapter is included in order to make this text self contained by providing an overview of subjects that are used in various applications later in the text. In particular, it aims to supplement the elementary view of radiation–matter interaction as a time-dependent perturbation in the Hamiltonian, by describing some aspects of the quantum nature of the radiation field. This is done on two levels: The main body of this chapter is an essentially qualitative overview that ends with a treatment of spontaneous emission as an example. The Appendix gives some more details on the mathematical structure of the theory. In elementary treatments of the interaction of atoms and molecules with light, the radiation field is taken as a classical phenomenon.
In this book we treat the interaction of radiation with matter with special application to gain (amplifying) media typically existing in lasers. Tradition ally the interaction of radiation with matter is treated in terms of the index of refraction and the absorption of light, utilizing the model of electrons on springs. In Chap. 3 we show that this model is reasonable for some linear absorbing systems but is very awkward, if not outright unworkable, for a microscopic description of gain media. The essential failure of the electron-spring model is its difficulty in yielding net stimulated emission (and therefore gain) for an ensemble of systems.t In contrast, a more physically sound, quantum treatment of matter provides for the concept of population inversion and explains stimulated emission in a natural way. Hence from the very start we are compelled to base our understanding of the interaction of radiation with matter on a quantum-mechanical description of atoms. In Chaps. 1-13 a classical field interacts with quantum-mechanical atoms; in the remainder of the book, both field and atoms are treated quantum mechani cally.
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.
The basic phenomena of interaction between atoms and e.m. fields can be discussed in some detail without the need of a detailed model of the atom. Absorption and stimulated emission of radiation can be explained satisfactorily by the theory, where a classical electromagnetic wave provides a time-dependent perturbation to the energy of the atomic electrons. Laser radiation appears to a very good approximation to be a classical travelling wave of well-defined amplitude and phase. The radiation produced by a continuous laser is a good approximation to a coherent state. For conventional sources of radiation, the interaction energy is small compared with the energy an electron possesses by virtue of the attraction to the atomic nucleus, so perturbation theory produces quite acceptable results. The quantum mechanical analogy to the distortion of the classical charge cloud is given by the writing down of a general state function for the system, Ψ.