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International Conference on Luminescence - 1984

A Novel Mechanism for Energy Transfer between Rare Earth Ions

W. Stręk

Published Jan 1, 1984• 0 citations
Publisher

Abstract

The theoretical understanding of resonant energy transfer between a pair of spatially localized lanthanide ions has been developed by Kushida [1]. His model was based on a simple application of Förster-Dexter theory [2,3] in which the transition rate of dipole-dipole energy transfer from the initial state | Dα Aβ > to the final state |Dα Aβ′> is proportional to the square of of modulus of where R is the separation between the donor - D and the acceptor - A ions.

DOI
10.1364/icol.1984.thd2

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The theoretical understanding of resonant energy transfer between a pair of spatially localized lanthanide ions has been developed by Kushida [1]. His model was based on a simple application of Förster-Dexter theory [2,3] in which the transition rate of dipole-dipole energy transfer from the initial state | Dα Aβ > to the final state |Dα Aβ′> is proportional to the square of of modulus of where R is the separation between the donor - D and the acceptor - A ions.
Estimations are made of the critical concentration of energy-acceptor ions for which the average efficiency of the excitation transfer from energy-donor ions is 1/2. This gives a measure of the activator concentration at which Inokuti and Hirayama's theory is no longer applicable. Study is also made of the dominant multipole interaction responsible for the energy transfer between rare earth ions in inorganic solids. Finally, importance of the J -selection rule in the determination of the dominant interaction term in the resonance transfer and cooperative processes is emphasized.
The rates of exciton transfer within dyads of perylene diimide and terrylene diimide connected by oligophenylene bridge units have been shown to deviate significantly from those of Förster's resonance energy transfer theory, according to single molecule spectroscopy experiments. The present work provides a detailed computational and theoretical study investigating the source of such discrepancy. Electronic spectroscopy data are calculated by time-dependent density function theory and then compared with experimental results. Electronic couplings between exciton donor and acceptor are estimated based on both transition density cube method and transition dipole approximation. These results confirm that the delocalization of exciton to the bridge parts contribute to significant enhancement of donor-acceptor electronic coupling. Mechanistic details of exciton transfer are examined by estimating the contributions of the bridge electronic states, vibrational modes of the dyads commonly coupled to both donor and acceptor, inelastic resonance energy transfer mechanism, and dark exciton states. These analyses suggest that the contribution of common vibrational modes serves as the main source of deviation from Förster's spectral overlap expression.
Accurate information on the distance dependence of resonance energy transfer (RET) is crucial for its utilization as a spectroscopic ruler \re{of} nanometer scale distances. In this regard, understanding the effects of donor-acceptor quantum coherence and non-Markovian bath, which become significant at short distances, has significant implications. The present work investigates this issue theoretically by comparing results from a theory of coherent RET (CRET) with a nonequilibrium version of Förster's RET (FRET) theory, both accounting for non-Markovian bath effects. Even for a model where the donor-acceptor electronic coupling is of transition dipole interaction form, it is shown that the RET rate in general deviates from the inverse sixth power distance dependence as opposed to the prediction of the original FRET. It is shown that the donor-acceptor quantum coherence makes the \re{distance} dependence steeper than the sixth power although detailed manner of enhancement is sensitive to specific values of parameters. On the other hand, the non-Markovian bath effects make the \re{distance} dependence more moderate than the sixth power for both CRET and nonueqilibrium FRET because finite time scale of the bath causes the rate to be smaller than the prediction of original FRET. While these effects are \re{demonstrated clearly} in the population dynamics at sub-picosecond time scales, their contributions to the conventional RET efficiency are relatively minor. This indicates that the actual detection of such effects through conventional RET efficiency measurement requires either high precision or utilization of a donor with fast spontaneous decay rate of excitation.