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Physical Review A

Interference between radiative emission and autoionization in the decay of excited states of atoms

Lloyd Armstrong, Constantine E. Theodosiou, Magnus Wall

Published Dec 1, 1978• 75 citations
Publisher

Abstract

An excited state of an atom which can autoionize can also undergo radiative decay. We consider the interaction between the final states resulting from these two modes of decay, and its effects on such quantities as the fluorescence yield of the excited state, excitation profile of the excited state, and the spectra of the emitted photons and electrons. It is shown that the fraction of decays of the excited state resulting in a photon (fluorescence yield) is particularly sensitive to the details of the final-state interaction. In lowest order in the final-state interaction, the fluorescence yield is increased by a factor $(1+\frac{1}{{q}^{2}})$ from the traditional value, where $q$ is the Fano $q$ parameter relating to the excited state and the final atomic state.

DOI
10.1103/physreva.18.2538

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Physical Review A•Aug 1, 1970•28 citations
An excited state of an atom which can autoionize can also undergo radiative decay. We consider the interaction between the final states resulting from these two modes of decay, and its effects on such quantities as the fluorescence yield of the excited state, excitation profile of the excited state, and the spectra of the emitted photons and electrons. It is shown that the fraction of decays of the excited state resulting in a photon (fluorescence yield) is particularly sensitive to the details of the final-state interaction. In lowest order in the final-state interaction, the fluorescence yield is increased by a factor (1+1q2)(1+\frac{1}{{q}^{2}})(1+q21​) from the traditional value, where qqq is the Fano qqq parameter relating to the excited state and the final atomic state.
The fluorescence produced by an autoionizing state under strong pumping by a coherent laser field is considered. It is shown how the spectrum of emitted photons and the total number of photons are related to the two-time and single-time atomic expectation values, and explicit expressions are derived for them. Numerical results for the time development of the number of photons ejected are presented for finite times and in the long-time limit. The photon spectra are shown to exhibit ac Stark splitting of the states involved. The spectrum is a doublet for transitions to a stable final state and a triplet for transitions connected back to the initial, strongly driven state. The decay of an autoionizing state in the absence of a laser driving field is considered, and the square of the Fano qqq value is interpreted as the ratio of two decay rates.
A theory describing the radiative decay of an autoionizing state under strong pumping by a coherent field is developed. The theory systematically takes into account the radiative decay of the unperturbed continuum. The problem at hand corresponds to the case of strongly coupled bound states decaying to electron and photon continua with the two continua also weakly coupled to each other. A master equation describing the time evolution of the atomic system is derived, and its exact solution under arbitrary initial conditions is given. The effect of radiative decay on the Fano profiles and photoelectron spectra is analyzed in detail. The time development of the system is also examined. The radiative decay of the autoionizing state and the unperturbed continuum changes the spectra in a significant way. The characteristics of the spectra are correlated with the dressed states (with complex energies) of the system. The changes in the structure of the dressed states as a function of the system parameters such as the spontaneous-emission rate and laser intensity are discussed in detail.
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.
In this paper we present a study of the radiative decay of coherently excited, closely spaced, molecular (or atomic) levels. Interference effects in the decay process cannot be treated in general by displaying the damping matrix in a diagonal form, so that each decay channel is assumed to be characterized by its own lifetime. The problem of the radiative decay of coherently excited indistinguishable levels (characterized by the same symmetry) is treated by a self-consistent extension of the Wigner-Weisskopf method, or alternatively, by the ‘unitarity relations’ method, developed in elementary particles physics. Finally, the Fano configuration interaction method is applied for the decay of a manifold of states characterized by the same polarization. General expressions for photon counting rates are derived and the nature of a general quantum beat experiment is discussed.
Spectral features of the radiation emitted by autoionizing states in the presence of a strong laser field are calculated under the condition of multiple photon absorption and emissions. The method is based on the exact solution of the master equation for the recycled system. The decay spectra are found to exhibit sharp maxima at the laser frequency and, for large values of the Fano qqq value, sidebands which are reminiscent of the triplet which one finds in the context of a two-level atom.
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.