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Molecular Physics

Interference effects in the radiative decay of closely spaced levels

Mordechai Bixon, Joshua Jortner, Yossef Dothan

Published Jan 1, 1969• 126 citations
Publisher

Abstract

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.

DOI
10.1080/00268976900100861

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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.
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.
Recent experiments (Dodd, Fox, Series & Taylor, I959; Colegrove, Franken, Lewis & Sands, i959) have shown that coherence effects can be observed between the Zeeman components of an optical line provided some coherence exists in the excited state. This coherence may be due to a radio-frequency field inducing transitions between the Zeeman sublevels of this excited state, or to the excitation process itself or to both. These effects are actually more or less a generalization of the well-known Hanle's experiments on the polarization of resonance radiation.: In the case of 'double resonance' experiments (Dodd et al. I959), they appear as a modulation of the intensity of the fluorescence radiation at one of the harmonics of the r.f. field; they can be interpreted as interference between the radiations of different frequencies emitted by the atoms which are submitted to the 'double resonance' ('light beat'). These coherence effects are related to those observed in the trapping of resonance radiation. In this paper, the methods used in former papers (Barrat I959 a, b and c, hereafter referred to as I, II, III) for the problem of light trapping are applied to the light beats experiments, using a density matrix formalism. The expression for the density matrix representing the states of the atoms just after the excitation will first be derived; then the intensity of the re-emitted light will be calculated. It will be shown finally how this method can be applied to practical problems. Notation unexplained in this paper is the same as in papers on coherence in light trapping (papers I, II and III).
We consider light scattering from a multilevel system (e.g., a molecule) interacting with several heat baths. The Liouville space approach is employed and weak incident radiation intensity is assumed, whereas the light scattering process is described in the lowest appropriate order in the interaction between the molecule and the incident and emitted photons. The interaction with other radiation field modes as well as with the thermal baths is treated more fully, such as to account for the correct damping terms and their temperature dependence. The formalism is suited for light scattering from an impurity molecule in both gas and dense phases. The thermal baths induce relaxation within the manifold of excited states as well as transitions to nonradiative channels. Damping due to such transitions (as well as radiative damping) corresponds to interactions with zero temperature baths. The physical interpretation of such a bath depends on the nature of the particular damping process. Thermal relaxation within the excited manifold is induced by interaction with the environment represented by a bath of temperature T. Part of this interaction which is diagonal in the molecular space corresponds to the so-called ’’quasielastic collisions’’ and induces modulations of the molecular energy levels and broadening of the relaxed emission. The remainder, nondiagonal part induces actual transitions between the excited molecular energy levels. The formalism yields in a single calculation expressions for the cross section for both the coherent (Raman) scattering process and the relaxed luminescence and enables us to discuss the effects of different factors such as temperature and quenching processes on the relative yields for these processes. The formalism also allows for interference between different levels of the excited manifold due to coupling of several levels to the same bath, and makes it possible to study the effect of thermal relaxation on these interference phenomena.
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.