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Physical Review

A Quantum Theory of Optical Phenomena

J. C. Slater

Published Apr 1, 1925• 24 citations
Publisher

Abstract

An attempt is made to present a consistent detailed theory of optical phenomena, based on the suggestion recently made by the author in collaboration with Bohr and Kramers. This suggestion is that atoms are radiating or absorbing continuously, during their stationary states, and that transitions influence radiation only in terminating the radiation characteristic of the old state, and substituting that of the new. The atoms, on the other hand, are supposed not to change their energy while radiating, but to change it discontinuously on transition. This necessitates giving up the detailed application of the conservation of energy in interaction between atoms and radiation. In the present paper, an additional suggestion is made, namely that resonance radiation is to be identified with the radiation carried out by the spherical wavelets which, by their interference with the external field, also produce absorption. This is practically a return to the classical picture of resonance radiation. Statement of the theory consists formally of two parts: the description of the behavior of atoms, and of radiation, when the two interact. The first involves the statement of the probabilities of transition of atoms, and is taken without change from Einstein. The probability of interruption of coherent vibrations is also discussed. The second requires the specification of the fields emitted by atoms in any steady state under the influence of any external field. These consist of spherical wavelets of the frequencies of the various quantum lines which the atom can emit or absorb in the stationary state in which it is. For emission frequencies, wavelets are emitted even in the absence of an external field; for absorption frequencies, external fields induce wavelets, similar to the wavelets of linearly bound electrons in electron theory, which on the one hand interfere with the external field to produce the phenomena of dispersion, etc., and on the other carry out the resonance radiation in all directions. Detailed descriptions of these fields are given. In a discussion of the theory, it is first shown that the assumptions which have been made about the field satisfy the correspondence principle, in that for large quantum numbers the field aproaches that which would be emitted classically on account of the interaction of an external field and a multiply periodic atom. On the other hand, it is shown that the field has a character essentially like that of classical electron theory, which is known to be in general agreement with experiments. Next, the energy and momentum relations at interaction of atoms and light are investigated, and it is shown that, although these quantities are not precisely conserved, still the assumptions as to atomic and radiation processes have been so made that they are conserved on an average over a great number of atomic processes. Finally the spectral resolution of emitted and absorbed radiation is considered; the theory gives a minimum breadth for the lines, depending on the finite length of wave trains resulting from the finite life in stationary states, and it is shown that Kirchhoff's law is obeyed, the emission and absorption lines being of the same breadth. By way of illustration, specific application of the theory is made to the simple examples of emission of light by bombardment of electrons at the resonance potential, resonance radiation, its quenching by presence of foreign gases, absorption, scattering, and disperison.

DOI
10.1103/physrev.25.395

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An attempt is made to present a consistent detailed theory of optical phenomena, based on the suggestion recently made by the author in collaboration with Bohr and Kramers. This suggestion is that atoms are radiating or absorbing continuously, during their stationary states, and that transitions influence radiation only in terminating the radiation characteristic of the old state, and substituting that of the new. The atoms, on the other hand, are supposed not to change their energy while radiating, but to change it discontinuously on transition. This necessitates giving up the detailed application of the conservation of energy in interaction between atoms and radiation. In the present paper, an additional suggestion is made, namely that resonance radiation is to be identified with the radiation carried out by the spherical wavelets which, by their interference with the external field, also produce absorption. This is practically a return to the classical picture of resonance radiation. Statement of the theory consists formally of two parts: the description of the behavior of atoms, and of radiation, when the two interact. The first involves the statement of the probabilities of transition of atoms, and is taken without change from Einstein. The probability of interruption of coherent vibrations is also discussed. The second requires the specification of the fields emitted by atoms in any steady state under the influence of any external field. These consist of spherical wavelets of the frequencies of the various quantum lines which the atom can emit or absorb in the stationary state in which it is. For emission frequencies, wavelets are emitted even in the absence of an external field; for absorption frequencies, external fields induce wavelets, similar to the wavelets of linearly bound electrons in electron theory, which on the one hand interfere with the external field to produce the phenomena of dispersion, etc., and on the other carry out the resonance radiation in all directions. Detailed descriptions of these fields are given. In a discussion of the theory, it is first shown that the assumptions which have been made about the field satisfy the correspondence principle, in that for large quantum numbers the field aproaches that which would be emitted classically on account of the interaction of an external field and a multiply periodic atom. On the other hand, it is shown that the field has a character essentially like that of classical electron theory, which is known to be in general agreement with experiments. Next, the energy and momentum relations at interaction of atoms and light are investigated, and it is shown that, although these quantities are not precisely conserved, still the assumptions as to atomic and radiation processes have been so made that they are conserved on an average over a great number of atomic processes. Finally the spectral resolution of emitted and absorbed radiation is considered; the theory gives a minimum breadth for the lines, depending on the finite length of wave trains resulting from the finite life in stationary states, and it is shown that Kirchhoff's law is obeyed, the emission and absorption lines being of the same breadth. By way of illustration, specific application of the theory is made to the simple examples of emission of light by bombardment of electrons at the resonance potential, resonance radiation, its quenching by presence of foreign gases, absorption, scattering, and disperison.
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.
Abstract The new quantum theory, based on the assumption that the dynamical variables do not obey the commutative law of multiplication, has by now been developed sufficiently to form a fairly complete theory of dynamics. One can treat mathematically the problem of any dynamical system composed of a number of particles with instantaneous forces acting between them, provided it is describable by a Hamiltonian function, and one can interpret the mathematics physically by a quite definite general method. On the other hand, hardly anything has been done up to the present on quantum electrodynamics. The questions of the correct treatment of a system in which the forces are propagated with the velocity of light instead of instantaneously, of the production of an electromagnetic field by a moving electron, and of the reaction of this field on the electron have not yet been touched. In addition, there is a serious difficulty in making the theory satisfy all the requirements of the restricted principle of relativity, since a Hamiltonian function can no longer be used. This relativity question is, of course, connected with the previous ones, and it will be impossible to answer any one question completely without at the same time answering them all. However, it appears to be possible to build up a fairly satisfactory theory of the emission of radiation and of the reaction of the radiation field on the emitting system on the basis of a kinematics and dynamics which are not strictly relativistic. This is the main object of the present paper. The theory is noil-relativistic only on account of the time being counted throughout as a c-number, instead of being treated symmetrically with the space co-ordinates. The relativity variation of mass with velocity is taken into account without difficulty. The underlying ideas of the theory are very simple. Consider an atom interacting with a field of radiation, which we may suppose for definiteness to be confined in an enclosure so as to have only a discrete set of degrees of freedom. Resolving the radiation into its Fourier components, we can consider the energy and phase of each of the components to be dynamical variables describing the radiation field. Thus if Er is the energy of a component labelled r and θr is the corresponding phase (defined as the time since the wave was in a standard phase), we can suppose each Er and θr to form a pair of canonically conjugate variables. In the absence of any interaction between the field and the atom, the whole system of field plus atom will be describable by the Hamiltonian H ═ ΣrEr + Ho equal to the total energy, Ho being the Hamiltonian for the atom alone, since the variables Er, θr obviously satisfy their canonical equations of motion Er ═ — ∂H/∂θr ═ 0, θr ═ ∂H/∂Er ═ 1.
Abstract The new quantum mechanics could at first be used to answer questions concerning radiation only through analogies with the classical theory. In Heisenberg’s original matrix theory, for instance, it is assumed that the matrix elements of the polarisation of an atom determine the emission and absorption of radiation analogously to the Fourier components in the classical theory. In more recent theories a certain expression for the electric density obtained from the quantum mechanics is used to determine the emitted radiation by the same formulæ as in the classical theory. These methods give satisfactory results in many cases, but cannot even be applied to problems where the classical analogies are obscure or non-existent, such as resonance radiation and the breadths of spectral lines. A theory of radiation has been given by the author which rests on a more definite basis. It appears that one can treat a field of radiation as a dynamical system, whose interaction with an ordinary atomic system may be described by a Hamiltonian function. The dynamical variables specifying the field are the energies and phases of its various harmonic conrponents, each of which is effectively a simple harmonic oscillator. One must, of course, in the quantum theory take these variables to be q-numbers satisfying the proper quantum conditions. One finds then that the Hamiltonian for the interaction of the field with an atom is of the same form as that for the interaction of an assembly of light-quanta with the atom. There is thus a complete formal reconciliation between the wave and light-quantum points of view.
‘At the present state of science it does not seem possible to avoid the formal character of the quantum theory which is shown by the fact that the interpretation of atomic phenomena does not involve a description of the mechanism of the discontinuous processes […]. On the correspondence principle it seems nevertheless possible to […] arrive at a consistent description of optical phenomena by connecting the discontinuous effects occurring in atoms with the continuous radiation field […]’. This announced a turning point in atomic physics research; for the first time there were reasons to assert that discontinuity was not in itself incompatible with the theory's descriptive content, and rational solutions were provided that related a whole set of phenomena dependent on the radiation properties of matter to the continuous picture of the radiation field. This was the conclusion arrived at in a new paper by Bohr which took up and developed the hypothesis put forward by the American physicist John Slater that ‘the atom, even before a process of transition between two stationary states takes place, is capable of communication with distant atoms through a virtual radiation field’ was taken up and developed. The article, ‘The Quantum Theory of Radiation’, signed by Bohr, Kramers and Slater, was published in the Philosophical Magazine in January 1924. Slater had arrived in Copenhagen at the end of the preceding year with the idea that his hypothesis might lead to very different theoretical results.
Introduction The preceding chapters have focused on atomic transitions induced by applied radiation. That is, there is an optical field illuminating the atoms, and their response is calculated. It is implicitly assumed that an excited atom left alone will spontaneously return to the ground state, and conserve energy by emitting light that satisfies E 2 − E 1 = ħ ω 21 in accordance with the Planck and Bohr pictures. But this spontaneous emission process is not addressed quantitatively in these earlier chapters. Spontaneous emission is one of the most pervasive phenomena of atomic physics, and yet its origins remain among the least well-understood. The number of misconceptions is enormous, and they are to be found in textbooks, journal articles, and lecture notes. Because the natural decay of an excited atom adds energy to what is usually an empty mode of the electromagnetic field, the process is fundamentally quantum mechanical. Classical or even semi-classical descriptions cannot be assured to give correct answers. This is not to say that such discussion is to be avoided, but only that caution is needed in interpreting the results. Toward the end of the nineteenth century, many experimental results made it clear that classical mechanics needed to be supplemented by new theories. The first venture into the new physics was Planck's hypothesis that the energy of classical radiating oscillators like those discussed in Chap. 1 would have to be quantized into integer multiples of ħ ω. This notion led to his famous formula for the spectrum of thermal radiation from a non-reflective object (black body), and this formula describes a radiation field in thermodynamic equilibrium with its environment. The result of Planck's hypothesis in the context of thermal equilibrium plays a vital role in the discussion of spontaneous emission. Einstein A - and B -coefficients Soon after Bohr proposed a model of atomic structure consisting of discrete energy levels, connected by radiation whose energy satisfied Δ E = ħω when atoms made transition between them, Einstein published the first serious attempt to connect the absorption and emission processes. Absorption, he reasoned, could occur only in the presence of applied radiation, whereas spontaneous decay occurred without the application of any field.
It is demonstrated that, if one remains in the framework of quantum mechanics taken alone, stationary states (energy eigenstates) are in no way singled out with respect to nonstationary ones, and moreover the stationary states would be difficult if possible to realize in practice. Owing to the nonstationary states any quantum system can absorb or emit energy in arbitrary continuous amounts. The peculiarity of the stationary states appears only if electromagnetic radiation that must always accompany nonstationary processes in real systems is taken into account. On the other hand, when the quantum system absorbs or emits energy in the form of a wave the determining role is played by resonance interaction of the system with the wave. Here again the stationary states manifest themselves. These facts and influence of the resonator upon the incident wave enable one to explain all effects ascribed to manifestation of the corpuscular properties of light (the photoelectric effect, the Compton effect etc.) solely on a base of the wave concept of light.