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Derivation of Einstein’s spontaneous emission coefficient with Schrödinger equation and classical electromagnetism

Ophelliam Loiselet

Published Jan 2, 2024• 0 citations
OpenAlex

Abstract

We will present here a clear derivation of the Einstein's spontaneous coefficient using Boudet's theory of probability transition current and classical electromagnetism. It is a step toward the quantum mechanics expressed in terms of real 3D fields quantities.

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Spontaneous emission

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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.

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Among theories of the physical world, quantum mechanics remains a topic of lively discussions on its so-called interpretation. For some it remains an open question to understand how deterministic equations of this theory, as established long ago, may combine with a fundamental uncertainty. We consider the process of spontaneous emission by an atom interacting with infinite number of degrees of freedom of the electromagnetic field. There is uncertainty in the evolution of the photo-emission process which was characterized as Markovian by using the equations of quantum mechanics when the decay of the atom is due to the coupling with the vacuum field. The Markovian property leads us naturally to describe spontaneous emission by using the classical Kolmogorov equation for the probability evolution of a parameter defining the state of the atom. We explain that Everett’s many-worlds interpretation weld together our description, and appears therefore as a consequence of the equations of quantum mechanics, that solves in this case the riddle of deterministic equations describing random events.

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Physical Review A•Aug 15, 2005•4 citations
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 has recently been shown by Jaynes and collaborators that semiclassical radiation theory contains a description of spontaneous emission of radiation and of radiative level shifts. The present paper gives a gauge-invariant derivation of the radiant energy production rate, using only Maxwell's equations and the usual definitions of electric current and charge density for a many-particle material system described by Schr\"odinger's equation. A complementary derivation, using the time-dependent Schr\"odinger equation, verifies the instantaneous conservation of energy and probability during the radiation process. The semiclassical rate of spontaneous emission differs from the usual formula (Einstein's AAA coefficient) because it depends on the occupancy of both initial and final states of the material system. The implications of this with regard to thermal equilibrium and Planck's law are examined. If a new hypothesis is introduced, postulating the decomposition of the equilibrium radiation into incoherent components, each interacting with a specific pair of energy levels of the material system, then Planck's law is shown to hold for the total intensity of radiation. If this hypothesis is not introduced, the equilibrium conditions for different transitions are incompatible, and the semiclassical radiation theory is incapable of describing thermal equilibrium.
Numerical simulations of stationary fluorescence spectra of molecular systems usually rely on the relation between the photon emission rate and the system’s dipole–dipole correlation function. However, research papers usually take this relation for granted, and standard textbook expositions of the theory of fluorescence spectra also tend to leave out this important relation. In order to help researchers with less theoretical training gain a deeper understanding of the emission process, we perform a step-by-step derivation of the expression for the fluorescence spectrum, focusing on rigorous mathematical treatment and the underlying physical content. Right from the start, we employ quantum description of the electromagnetic field, which provides a clear picture of emission that goes beyond the phenomenological treatment in terms of the Einstein A coefficient. Having obtained the final expression, we discuss the relation of the latter to the present level of theory by studying a simple two-level system. From the technical perspective, the present work also aims at familiarizing the reader with the density matrix formalism and with the application of the double-sided Feynman diagrams.
Among theories of the physical world, quantum mechanics remains a topic of lively discussions on its so-called interpretation. For some it remains an open question to understand how deterministic equations of this theory, as established long ago, may combine with a fundamental uncertainty. We consider the process of spontaneous emission by an atom interacting with infinite number of degrees of freedom of the electromagnetic field. There is uncertainty in the evolution of the photo-emission process which was characterized as Markovian by using the equations of quantum mechanics when the decay of the atom is due to the coupling with the vacuum field. The Markovian property leads us naturally to describe spontaneous emission by using the classical Kolmogorov equation for the probability evolution of a parameter defining the state of the atom. We explain that Everett’s many-worlds interpretation weld together our description, and appears therefore as a consequence of the equations of quantum mechanics, that solves in this case the riddle of deterministic equations describing random events.
The rate of spontaneous electromagnetic emission in a cavity is the normalized output radiation rate in the classical electrodynamics and the Einstein AAA coefficient in a quantum theory. We reveal the difference and similarity between the quantum and classical rates by calculations of the relative output power of the resonant spontaneous electric-dipole emission as a function of light absorption in a high-QQQ cavity. We show that the relative resonant output power is equal to the relative width of a morphology-dependent resonance in the spectral dependence of the Einstein AAA coefficient. The validity of the theory is demonstrated by numerical verification of an experimental result on a microsphere.