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Optics and Spectroscopy

Kinetics of nonstationary migration-accelerated energy transfer in a solid body doped with rare-earth and transition-metal ions

N. A. Glushkov

Published May 1, 2014• 1 citation
Publisher

Abstract

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.

DOI
10.1134/s0030400x14050099

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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.
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.
Summary form only given. The migration of excitation energy within dielectric crystals doped with lanthanide ions is a rich area for the study of mechanisms involving both conventional pairwise resonance energy transfer and more complex many-body effects. Within the framework of molecular quantum electrodynamics, we present a delineation of systems undergoing simultaneous transfer from two pre-excited donor ions to a single ground-state acceptor, termed three-centre energy pooling. Calculations lead to the identification of two competing mechanisms of transfer co-existing in each system-one cooperative pathway where the excitation is transferred directly to the acceptor from both donors, alongside an accretive mechanism where the excitation energy of one donor is accrued by a second, with net transfer to the acceptor ensuing.
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.