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Physical Review

Decay Modes with Coherent Resonant-Energy Transfer between Deep Impurities in Solids

Russell C. Casella

Published Oct 15, 1968• 5 citations
Publisher

Abstract

Attention is called to the existence of new decay modes for deep impurities in solids associated with coherence in the resonant-energy transfer between them. The theoretical decay rate $R$ of the two-impurity complex is of the form $R(t)={C}_{1}\mathrm{exp}(\ensuremath{-}{\ensuremath{\gamma}}_{1}t)+{C}_{2}\mathrm{exp}(\ensuremath{-}{\ensuremath{\gamma}}_{2}t)+\mathrm{exp}[\ensuremath{-}\frac{1}{2}({\ensuremath{\gamma}}_{1}+{\ensuremath{\gamma}}_{2})t]\ifmmode\times\else\texttimes\fi{}\mathrm{Re}D\mathrm{exp}(\ensuremath{-}i\ensuremath{\Delta}t)$, with ${C}_{n}$, ${\ensuremath{\gamma}}_{n}$ real positive, $\ensuremath{\Delta}$ real, and $D$ complex. The oscillations in time $t$ exhibited by the third term in the expression for $R$ provide an experimental test for the coherence effect. The partial rate ${R}_{\ensuremath{\nu}}(t)$ for radiative decay is of the same form as the total rate $R(t)$. In the analysis, use is made of an analogy between the decay of the excited impurity complex and that of ${K}^{0}$ mesons in particle physics, where similar coherent oscillations have been observed experimentally.

DOI
10.1103/physrev.174.830

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This study carries out an experimental investigation of the radiative decay kinetics of the resonance states of sodium atoms excited by dye laser radiation. The effective radiative decay rates of the resonance states as a function of vapor temperature, primary and impurity gas presssure, and the radius of the cylindrical volume containing the vapor were obtained by computer processing ofthe experimental curves using a kinetic decay model.-The radiative decay rate calculated in the Holstein approximation is compared to the measured values. The mechanisms of optical excitation of metallic vapors in resonance radiation trapping conditions have been investigated theoretically to a sufficient degree.lr At the same time there have been few experimental studies devoted to this problem. The decay kinetics of the atomic resonance states in the vapors of alkali metals have largely been studied for a planar radiating layer,2-6 where the nonideal geometry of the radiating volume made it necessary to introduce a fitting parameter to compare the experimental results to theory. The radiative decay kinetics of the populations of the resonance 3P states of atomic Na under conditions of axial laser excitation of a cylindrical shell are investigated in the present paper for the first time; this made it possible to carry out a comparison to theory without introducing variable parameters, since in this case exact analytic expressions are known for the effective lifetimes. It should also be emphasized that cylindrically configured cells are most commonly used in experimental research and hence these results have a certain interest in such studies. For our analysis we selected a concentration range of normal sodium atoms of 3 X 1013 <;no<;4 X 1015 cm - where selective optical excitation of the fine structure components (FSC) 32Pl/2 and 32P3/2 are accompanied by collisional mixing, which has a substantial effect on the persistence kinetics of the NaD lines. Under these conditions the decay of the directly excited fine structure component is biexponential, while the time dependence of the population of the corresponding level takes the form
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.
Summary form only given. Optical interactions in semiconductor microcavities embedded with quantum wells enter a nonperturbative regime when the dipole coupling rate between the exciton and the cavity mode exceeds relevant decay rates. In this regime, coherent energy exchange between the exciton and the cavity mode, i.e. normal mode oscillation (NMO), takes place when the cavity mode is excited impulsively by a short laser pulse. Similar coherent oscillations have also been observed in transient four-wave mixing (FWM) responses. In this paper, we present experimental and theoretical studies on the nature of oscillations in these transient FWM responses. We show that, in contrast to earlier beliefs, oscillations in time-integrated transient FWM do not correspond to NMO of the exciton or photon populations. Theoretical studies further reveal that FWM arising from different physical mechanisms including band filling, excitation-induced dephasing, and renormalized electric fields is characterized by highly distinct coherent dynamics. Oscillations in transient FWM reflect interference between these coherent optical processes and can be used as a unique probe for exciton many-body interactions in the nonperturbative regime.