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Physical Review A

Radiative Decay of Coupled Atomic States

Peter R. Fontana, Donald J. Lynch

Published Aug 1, 1970• 28 citations
Publisher

Abstract

The radiative decay of an atom with two excited states coupled by an external perturbation is investigated. The differential equations of motion are Fourier transformed and the probability amplitudes are obtained by contour integration. The real parts of the poles in the complex plane are the perturbed energies of the excited states, and the imaginary parts yield the decay characteristics. The decay probabilities of the excited states contain three different decay terms; two exponential decays and one modulated exponential decay. The probabilities of the final states give the frequency distribution of the emitted photons as a function of time. In an Appendix, the Heitler-Ma formalism is used to eliminate the final states of the system, and the resulting equations which contain damping terms are compared with the phenomenological method.

DOI
10.1103/physreva.2.347

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The radiative decay of an atom with two excited states coupled by an external perturbation is investigated. The differential equations of motion are Fourier transformed and the probability amplitudes are obtained by contour integration. The real parts of the poles in the complex plane are the perturbed energies of the excited states, and the imaginary parts yield the decay characteristics. The decay probabilities of the excited states contain three different decay terms; two exponential decays and one modulated exponential decay. The probabilities of the final states give the frequency distribution of the emitted photons as a function of time. In an Appendix, the Heitler-Ma formalism is used to eliminate the final states of the system, and the resulting equations which contain damping terms are compared with the phenomenological method.
The spontaneous radiative decay to the ground state of an atomic system initially in the higher of two excited states, coupled in a radiationless fashion by an external field, is investigated by the method of multiple-time-scale perturbation theory. The coupled differential equations of motion for the probability amplitudes are solved to second order, while the usual secular behavior of conventional time-dependent perturbation theory is eliminated in terms of two natural time scales: a fast time scale corresponding to the reciprocal of the level transition frequency and a slower time scale associated with the inverse of the radiation linewidth. Expressions are obtained to this order for the energy shifts and decay characteristics of the excited states and the energy distribution of the final-state photons, quantities previously determined by Fourier analysis and contour integration and by the phenomenological approach of Weisskopf and Wigner. A detailed comparison of these various methods of solution includes conditions under which the present results agree to second order with the previous calculations.
The excitation and decay probabilities for resonance scattering of radiation from an atom with two coupled excited states in an external static field are calculated as a function of time and frequency. Various oscillatory terms are found in the probabilities. These oscillations depend on the frequency of radiation, the external coupling and the energy difference between the excited states. Two special cases are investigated in detail. In the first case where one of the excited states does not decay a 'hole' appears in the emission line at a frequency equal to the frequency difference between the ground state and the unperturbed non-decaying excited state. In the second case where the two excited states decay with the same rate, one of the two lines in the emission spectrum is suppressed and the other is enhanced.
A critical examination of the theory of resonance radiation has been carried through, employing the mathematical technique of Laplace and Stieltjes transforms. Particular attention has been devoted to the question of the temporal behavior of the excited state. With no restrictions on the interaction between atom and radiation field other than that it be real, and that processes of sufficiently high frequency contribute only negligible effects, one can prove that the probability amplitude of the excited state cannot decay according to the general law ${\ensuremath{\Sigma}}_{\ensuremath{\mu},\ensuremath{\nu}}{C}_{\ensuremath{\mu}\ensuremath{\nu}}{t}^{{\ensuremath{\lambda}}_{\ensuremath{\mu}}}{e}^{\ensuremath{-}{\ensuremath{\beta}}_{\ensuremath{\nu}}t},$ where the ${\ensuremath{\lambda}}_{\ensuremath{\mu}}$ and ${\ensuremath{\beta}}_{\ensuremath{\nu}}$ are complex constants lying in the right half-plane and the ${C}_{\ensuremath{\mu}\ensuremath{\nu}}$ are arbitrary complex coefficients. The deviation from the law just cited can be termed a straggling phenomenon since exact analysis shows that the probability amplitude, for sufficiently long times, is greater than that defined according to the radioactive decay law.Rigorous analysis of the source of this apparently anomalous behavior reveals the following explanation. Although the probability amplitude of the excited state is, strictly speaking, a functional of the interaction between the transition current in the atom and the photon states of the electromagnetic field, the essential features are determined principally by those states lying near the resonance frequency. Three elementary observations are immediately apparent. First, a particularly tractable analytical approximation for the interaction can be made such that the value of the actual interaction is reproduced at the resonance frequency and such that the behavior for high and low frequency photon states is at least qualitatively correct. Exact solutions in closed form can be obtained for this interaction. Second, in terms of the preceding representation it is possible to show that, associated with the transition between two atomic states, one is presented with a concomitant picture of a damped oscillation of charge describable in purely classical terms. Third, this classical motion can be interpreted as forming a source function for a continuous stochastic process in terms of which one finally derives the representation of the probability amplitude of the excited state. The straggling phenomenon previously cited is therefore that associated with all diffusion processes. The consideration of the exact interaction leads to more involved diffusion phenomena but does not in any case permit a radioactive decay law.
A two-level atom interacting simultaneously with an external static field is reinvestigated. Here, first the Hamiltonian of the atom and the external field is diagonalized and then the interaction of the radiation field is considered. This method yields, directly, the state populations for the atom, and the lineshape and linewidth of the spontaneously emitted radiation. The earlier result on the state populations by Bali and Higgins has been compared with the present work and found to be in good agreement. The line shape of the emitted radiation is Lorenzian and the halfwidth is found to be increasing with increasing external perturbation. For the case where the atom is initially in the excited state, the intensity of the emitted radiation decreases with increasing perturbation and finally reaches a saturation limit. However, when the atom is considered to be in the ground state, initially, the intensity increases with increasing perturbation and it again reaches a saturation limit at a large perturbation field.
We examine the exponential decay law for an excited quantum system in the case where the state amplitude has a “memory,” that is, where the rate at which the amplitude is decaying at a particular time depends to some extent on values of the amplitude at previous times. For a particular choice of memory, characterized by a memory time τ, the amplitude obeys the differential equation of a damped harmonic oscillator. When τ is greater than a certain critical memory time τc, comparable to the natural lifetime of the state, the amplitude becomes an exponentially damped oscillation in time. When τ is less than τc, the decay is nearly exponential with a decay rate somewhat greater than that calculated from standard theory. By comparing theory with experiment, we can place an upper limit on the memory time for the radiative decay of atoms.
In this paper we analyze the dynamics of single-excitation states, which model the scattering of a single photon from multiple two level atoms. For short times and weak atom-field couplings we show that the atomic amplitudes are given by a sum of decaying exponentials, where the decay rates and Lamb shifts are given by the poles of a certain analytic function. This result is a refinement of the "pole approximation" appearing in the standard Wigner-Weisskopf analysis of spontaneous emission. On the other hand, at large times, the atomic field decays like O(1/t3)O(1/t^3)O(1/t3) with a known constant expressed in terms of the coupling parameter and the resonant frequency of the atoms. Moreover, we show that for stronger coupling, the solutions also feature a collection of oscillatory exponentials which dominate the behavior at long times. Finally, we extend the analysis to the continuum limit in which atoms are distributed according to a given density.