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Advanced Solid-State Lasers

Cooperative Quenching Energy Transfer in La1−xCexF3 Crystal

Tasoltan T. Basiev, Maxim E. Doroshenko, В. В. Осико

Published Jan 1, 2000• 1 citation
Publisher

Abstract

A new phenomena of nonradiative cooperative energy transfer from optically excited single Nd3+ ion to the cooperative acceptor formed by a pair of Ce3+ ions and from single excited Er3+ ion simultaneously to three Ce3+ ions acting as a nonlinear cooperative acceptor was observed by measuring the concentrational quenching of donor ions fluorescence in solid solution of La1−xCexF3.

DOI
10.1364/assl.2000.mb12

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A new phenomena of nonradiative cooperative energy transfer from optically excited single Nd3+ ion to the cooperative acceptor formed by a pair of Ce3+ ions and from single excited Er3+ ion simultaneously to three Ce3+ ions acting as a nonlinear cooperative acceptor was observed by measuring the concentrational quenching of donor ions fluorescence in solid solution of La1−xCexF3.
Summary form only given. We report on a new nonlinear optical phenomenon in LaCeF/sub 3/:Nd crystals of cooperative energy transfer-cooperative cross-relaxation, that is the energy transfer from single donor ion simultaneously to the pair (or more) ions, acting as nonlinear cooperative acceptor. The dependence of fluorescence intensity and decay rate at the kinetic stage of the process here can not be described by linear dependence on acceptor's concentration and becomes essentially nonlinear.
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.
Up to now, only quantum computing using few quantum bits have been realized [1]. Main obstacles to increase the size of quantum register are fast decoherence and difficulties to control many-qubits entanglement. The clusters of the Nd3+ions formed in the Nd3+:LaF3crystal can be a candidate for many-qubit CNOT-gate, because of their entangled states due to strong coherent interaction (Davydov's splitting; bright and dark states with their own lifetimes τ and ra), weak electron-phonon coupling and long coherence time of the excited states. It was shown earlier that satellite lines of the main spectral line for single-site optical center of absorption [2, 3] and fluorescence excitation spectra [2] of Nd3+:LaF3crystals can be attributed to Nd3+ion pairs. The direct measurement of the fluorescence decay times for various classes of Nd3+pairs was made [2] since the pairs are well selected by fluorescence excitation wavelength.
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 transfer of energy from single chromium ions to closely coupled pairs of chromium ions in ruby has been investigated. Ruby samples whose concentrations ranged from 0.003 to 1.0% Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​ were prepared and in each crystal the intensity of single-ion fluorescence and of pair fluorescence was accurately measured. Radiative-decay measurements were also made in an attempt to unravel the dynamics of the transfer process. The transfer from single ions to pairs is shown to occur nonradiatively, and its efficiency is enhanced by a fast energy transfer between individual single ions. The possibility is explored that an electric quadrupole-quadrupole interaction is responsible for this transfer process.