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Journal of Applied Spectroscopy

Analysis of fluorescence decay in the presence of a continuous distribution of emitters with repsect to lifetime

Alexander A. Maskevich, S. K. Basharin, Gennedy A. Gachko, Leonid N. Kivach, С. А. Маскевич

Published Oct 1, 1990• 1 citation
Publisher
DOI
10.1007/bf00662610

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Photonic crystals (PCs) with relatively low dielectric contrast (i.e., with pseudogaps) have significant influence on the fluorescence decay of internal emitters. Fluorescence decays of ensembles of dye molecules measured at different positions in the PCs exhibit a nonexponential behavior, which is best fitted by a continuous distribution of decay rates. The most frequent decay rates of these distributions are smaller and their widths are narrower in a PC with a pseudogap acting in the emission range of the emitters than in a PC having the pseudogap out of this range. These experimental results have been well accounted for by calculations of the local density of states and rate constant for spontaneous emission.
In this work we expose a recently developed theoretical model for the analysis of the measurements obtained with the so-called pinhole method, for the determination of the upper level lifetime in materials where the superimposition between fluorescence and absorption spectra determines significant radiation trapping effect. Under fairly general conditions the fluorescence decay curve after a pulsed excitation of the sample obtained with this experimental set-up can be conveniently described by a double exponential functional form. The faster of the two decay times is close to the intrinsic fluorescence lifetime, with a difference that can be calculated with geometrical considerations. The theoretical results were tested with a suitably designed experiment, where the upper level lifetime of the laser transition of some Yb doped samples were investigated, obtaining results that are consistent with literature data and in good agreement with the theoretical results as for the temporal dependence of the fluorescence decay.
We investigate the quantum Zeno effect in the case of electron tunneling out of a quantum dot in the presence of continuous monitoring by a detector. It is shown that the Schr\"odinger equation for the whole system can be reduced to Bloch-type rate equations describing the combined time development of the detector and the measured system. Using these equations we find that continuous measurement of the unstable system does not affect its exponential decay to a reservoir with a constant density of states. The width of the energy distribution of the tunneling electron, however, is not equal to the inverse lifetime---it increases due to the decoherence generated by the detector. We extend the analysis to the case of a reservoir described by an energy-dependent density of states, and we show that continuous measurement of such quantum systems affects both the exponential decay rate and the energy distribution. The decay does not always slow down, but might be accelerated. The energy distribution of the tunneling electron may reveal the lines invisible before the measurement.
In quantum mechanics, the properties of an unstable system are closely related to its corresponding energy distribution. One of the predictions of the theory is the emergence of a late-time power law in the survival probability P(t)P(t)P(t) of the unstable state. However, in complex systems, similar effects may emerge due to other phenomena. This is the case for nonextensive statistical models, for some continuous lifetime distribution models, and also for certain energy-migration models applied to fluorescence. In this work, these alternative interpretations are confronted with data from time-resolved fluorescence spectroscopy experiments with erythrosine B and eosine Y as fluorophores. It turns out that some of the features expected within the quantum-mechanical description, such as the sharp transition from the exponential to the power-law regime, cannot be reproduced by the specific statistical and energy-migration parametrizations fitted in the analysis.