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Physical Review

A General Solution for the Equations of Natural Line Breadth

Lyman Spitzer

Published Feb 15, 1939• 14 citations
Publisher

Abstract

A rigorous solution is given to the Dirac radiation equations for a single radiative transition between two atomic states. The resultant formulas are valid for any appropriate variation with frequency both of the density of light quanta and of the matrix component for the transition. The usual infinity at high frequencies is eliminated naturally. Applications of the formulas are made for the case of an absorption or an emission line.

DOI
10.1103/physrev.55.361

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•Jan 1, 1974•0 citations
A rigorous solution is given to the Dirac radiation equations for a single radiative transition between two atomic states. The resultant formulas are valid for any appropriate variation with frequency both of the density of light quanta and of the matrix component for the transition. The usual infinity at high frequencies is eliminated naturally. Applications of the formulas are made for the case of an absorption or an emission line.
Abstract A general and exact formalism is developed that permits the calculation of the line shape in all line-breadth phenomena, in principle to any order of approximation. Expansions for the line breadth and the numerator occurring in the line-shape formula are given. Corrections to the classical line shape include: (i) radiative corrections to the line breadth, (ii) a level shift additional to the usual radiative shift for levels with finite transition probability, (iii) radiative corrections to the numerator and (iv) a slight frequency dependence of the numerator. All these corrections, with the exception of (iv), are exceedingly small. The case of radio-frequency transitions is discussed.
A method for obtaining the intensity distribution in a spectral line is derived from Dirac's quantum theory of the radiation field. The calculations are carried out for the case of emission from a first excited state (resonance line) and show that the intensity of frequency $\ensuremath{\nu}$ is, in this case, proportional to $\frac{1}{[4{\ensuremath{\pi}}^{2}{({\ensuremath{\nu}}_{0}\ensuremath{-}\ensuremath{\nu})}^{2}+{(A\ifmmode\cdot\else\textperiodcentered\fi{}2)}^{2}]}$ were AAA is the rate at which atoms are leaving the upper state and ${\ensuremath{\nu}}_{0}$ is the frequency of the transition. The half-width is therefore $\frac{1}{2\ensuremath{\pi}}$ times the Einstein probability coefficient for spontaneous transition to the lower state. The more general case where the lower state has a finite life time is not treated.A general method for the treatment of radiation problems, which is essentially Weyl's modification of Dirac's method, is briefly described.
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.
Abstract The calculations of the preceding chapter display some of the inadequacies of the Einstein theory of interaction of light with atoms. The theory itself gives no prescription for computing the values of the A and B coefficients appropriate to a given atomic transition. For this one must look to the quantum-mechanical theory of transition probabilities. As light beams are generated by emission from atoms and measurements on light beams ultimately depend on the absorption of light by atoms, it is essential to cover the theory of the atomic interaction processes, even though the main interest of the book is the quantum nature of the light itself. More seriously, the Einstein theory is applicable only for broad-band illumination of the atom, where the energy in the incident light is distributed smoothly across the frequencies within the linewidth of the atomic transition. By contrast, many experiments with laser sources use light beams whose frequency distributions are much narrower than atomic transition linewidths.
Several calculations have been carried out using the transition operator technique. The radiative decay in a two-level quantum system with excited state coupled by an external perturbation has been investigated and an expression obtained for P(t), the probability of finding the atom in its excited state at time t. This is seen to possess a steady value for yt >> 1 and a third term which decays at nearly half the rate of its second. Next radiative decay of an atom with two close-lying excited states is considered and |bq| 2 , the spectral density for spontaneous emission from the uppermost level, calculated. This shows that the proximity of the upper two levels makes the line-shape non-Lorentxian. Heisenberg equations of motion were then derived for the transitions operators of an ℓ-level atom undergoing radiative decay, the possibility of overlapping pairs of levels being ignored. These master equations were then used to obtain the spectral profiles of certain atomic lines, employing the so-far avoided Markoff approximation. First the spectral density of the scattered radiation was found for transitions between levels 5P3/2 and 4S (ground state), and 6S and 5P 3/2, in the potassium atom when driving fields of arbitrary strength coupled levels 6S and 4P3/2, and 4P 3/2 and 4S. Triple-peaked profiles were obtained. Spectral profiles for emission were then derived for transitions between levels 3P and (ground state), and 3P and in the hydrogen atom when a driving field of arbitrary strength coupled levels The former profile was double the latter quadruple-peaked. Lastly master equations were derived for an atom, with two excited levels undergoing radiative decay, when allowance was made for thepossibility of their overlapping. A driving field of arbitrary magnitude coupled the uppermost and ground states. The spectrum for the scattered light resulting from transitions between the uppermost and ground state was found and graphs computed for various field strengths and separations of the excited states.