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Physical Review A

Multiple-time-scale perturbation theory: Radiative decay of coupled atomic states

G. L. Brooks, Leonard M. Scarfone

Published Dec 1, 1982• 4 citations
Publisher

Abstract

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.

DOI
10.1103/physreva.26.3268

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Journal of Physics B Atomic and Molecular Physics•Jun 1, 1974•3 citations
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.
In this first article of work on radiation processes, a multiple-time-scale expansion method specifically for these processes is developed, based on the two distinct time scales corresponding to the natural frequency and the linewidth of the radiation. The method is then demonstrated by treating systems of one and two two-level atoms. It is seen that the exponential-decay behavior of the excited-state amplitude, assumed a priori by Weisskopf and Wigner, follows naturally from the mathematical procedure of eliminating the secularity in each order of the expansion. The results of two-atom systems also agree with those of previous workers.
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 multiple-linear-time-scale method is used to construct a perturbation theory for NNN-level quantum systems subjected to time-dependent perturbations. The secular and small-denominator terms which plague conventional time-dependent perturbation theory are avoided; consequently, the theory is useful for treating long-term behavior and resonant interactions. The introduction of a self-energy operator allows the shifts in energy levels to be displayed explicitly. When the perturbation is the dipole interaction with an electromagnetic field, the successive approximations yield the well-known rotating-wave approximation, corrections due to counter rotating terms, and the Bloch-Siegert frequency shift. The formalism is applicable to arbitrary pulse shapes, provided that $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}\ensuremath{\ll}\ensuremath{\hbar}\overline{\ensuremath{\omega}}$, where $\ensuremath{\parallel}{H}_{1}\ensuremath{\parallel}$ represents the inter-action strength and $\overline{\ensuremath{\omega}}$ is a characteristic frequency of the field. Rabi oscillations induced by multiphoton resonances are automatically included, and this effect is demonstrated in the case of a square pulse with frequency approximately one half the resonance frequency for a transition between two vibrational levels of a molecule. These calculations are compared to an exact numerical solution in order to find the limits of validity of the approximation. Even at high intensities ($I\ensuremath{\sim}{10}^{14}$ W/cm2{\mathrm{cm}}^{2}cm2) the shifted resonance frequency is quite accurate; however, the approximate and exact solutions are slightly out of phase, so that the approximate solution can only be trusted for a few Rabi cycles. For much lower intensities ($I\ensuremath{\sim}{10}^{10}$ W/cm2{\mathrm{cm}}^{2}cm2), the approximate solution is valid for many thousands of Rabi cycles.
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.
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.
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.