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Soviet Journal of Quantum Electronics

Transfer of excitation energy between trivalent rare earth ions in crystals

Georgii M. Zverev, I. I. Kuratev, А. М. Онищенко

Published Mar 31, 1975• 0 citations
Publisher

Abstract

An analysis is made of the transfer of the excitation energy between trivalent rare earth ions in crystals. The multipole interaction mechanisms are considered and allowances made for the migration of the excitation energy between donor ions. The proposed model is used in estimating the probabilities of elementary energy transfer events, diffusion coefficients of excitations, and concentrations of quenching centers in the case of several rare earth ions in Y3Al5O12. A comparison is made of the experimental and calculated concentration and temperature dependences of the transfer of the excitation energy between trivalent rare earth ions in Y3Al5O12 crystals; the agreement between the calculations and the experiment is good.

DOI
10.1070/qe1975v005n03abeh010966

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An analysis is made of the transfer of the excitation energy between trivalent rare earth ions in crystals. The multipole interaction mechanisms are considered and allowances made for the migration of the excitation energy between donor ions. The proposed model is used in estimating the probabilities of elementary energy transfer events, diffusion coefficients of excitations, and concentrations of quenching centers in the case of several rare earth ions in Y3Al5O12. A comparison is made of the experimental and calculated concentration and temperature dependences of the transfer of the excitation energy between trivalent rare earth ions in Y3Al5O12 crystals; the agreement between the calculations and the experiment is good.
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 This gives a measure of the activator concentration at which Inokuti and Hirayama's theory is no longer applicable.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.
Calculations made of the rates for several processes involving interactions between rare earth ions in crystals, such as resonance energy transfer, cooperative excitation transfer and cooperative optical transitions. These processes are assumed to originate from the electric multipole interactions between the ions concerned. A tensor operator method is employed in order to take account of the individual characters of the energy levels involved in the transition. Evaluation of the typical transition probability is also made on the lowest-order parity-allowed processes in nearest neighbour ions. The rates for the resonance transfer and cooperative transfer processes thus estimated are much smaller than those obtained by Miyakawa and Dexter.
The kinetics of migration-accelerated energy transfer is studied in systems based on a massive crystal and a sample consisting of spherical nanoparticles up to and including four or five orders of magnitude of the kinetic expulsion depth for the case of donor excitation by a short (τpulse < τ D ) pulse under the action of a multipole mechanism of donor-donor and donor-acceptor energy transfer. The susceptibility of the chosen systems to the implementation of the “jump” mechanism of excitation transfer in them is estimated. It is shown that the nonstationary mechanism of excitation transfer is implemented in the chosen systems based on a sample consisting of nanoparticles.
The time and temperature dependences of the probability of deactivation of the excited state of the Yb 3+ ions in mixed yttrium-ytterbium garnets of various compositions were investigated in the temperature range 1.7–300°K. An analysis indicated that these dependences were governed by the excitation energy migration, which was the "bottleneck" in the process of nonradiative deactivation of the excited state. A strong rise (by more than an order of magnitude) of the migration probability was observed when the temperature was raised from 1.7 to 4.2°K. The diffusion theory, applicable to migration processes in the case of homogeneous broadening of spectral lines, was generalized to inhomogeneous broadening. The theoretical results were in good agreement with the experimental data.
We have investigated the possibility of realizing a 4-center energy transfer among trivalent rare Earth ions in suitable hosts. A 4-center energy transfer process was originally proposed in the context of photo-physics of dendrimer molecular systems using molecular quantum electrodynamics methods. Later, a similar theoretical construct was proposed for rare Earth ions in crystalline solids. Here, we search for rare Earth ions suitable for 4-center energy transfer based on observed energy levels of 4f n multiplet structures in suitable hosts. A search for this 4-center cooperative energy transfer process experimentally will open a novel area of research in luminescence.