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Quantum Electronics and Laser Science Conference

Nonlinear cooperative energy transfer in La/sub 1-x/Ce/sub x/F/sub 3/ crystals

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

Published May 12, 2000• 0 citations
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Abstract

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.

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Trapping of optical excitation by two types of acceptors in La0.72 Pr0.25 Nd0.03 F3

Thomas J. Glynn, I. Laulicht, Liren Lou +2 more

We have investigated the process of quenching of fluorescence from the $^{3}P_{0}$ state of ${\mathrm{Pr}}^{3+}$ in ${\mathrm{La}}_{0.72}$${\mathrm{Pr}}_{0.25}$${\mathrm{Nd}}_{0.03}$${\mathrm{F}}_{3}$ due to cross relaxation to Pr and Nd ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature in the (2-70)-K region. Cross relaxation occurs either directly or through a donor-donor transfer within the inhom-geneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from previous fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint according to models for fluorescence decay in the presence of traps. In general the decay is consistent with an electric dipole-dipole transfer mechanism. At 2 K the decay can be well described by a direct transfer to Pr and Nd traps without donor-donor transfer. The temperature dependence of the decay at long times can be described for $35<T<70$ K by the hopping model. The agreement with theory is much better if the cross relaxation to Nd ions is assumed to occur mainly via the lowest Stark level of the $^{4}I_{\frac{9}{2}}$ manifold.

Physical review. B, Condensed matter•May 1, 1984•9 citations
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.
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.
We report the discovery of population in the 1S0^{1}S_{0}1S0​ state (46 986 ${\mathrm{cm}}^{\ensuremath{-}1}$) of Pr3+{\mathrm{Pr}}^{3+}Pr3+ following the excitation of the 3P0^{3}P_{0}3P0​ state (20 925 ${\mathrm{cm}}^{\ensuremath{-}1}$) by a 477.8-nm pulse laser. The energy upconversion is attributed to a cooperative energy transfer from a pair of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions in the 3P0^{3}P_{0}3P0​ state to a nearby ion in the same state. A PrF3{\mathrm{F}}_{3}F3​ crystal and three LaF3{\mathrm{F}}_{3}F3​:Pr3+{\mathrm{Pr}}^{3+}Pr3+ crystals doped with 10, 20, and 60 at.% Pr3+{\mathrm{Pr}}^{3+}Pr3+ are tested in our experiment. The lifetime of the 1S0^{1}S_{0}1S0​ state and the decay of the 3P0^{3}P_{0}3P0​ state of each of the crystals are investigated. The results are used to solve the rate equations for calculating the temporal variations of the populations in the 1S0^{1}S_{0}1S0​ state in different crystals. The calculated result agrees with the measured variation of the uv emission ($^{1}S_{0}\ensuremath{\rightarrow}^{3}P_{1}+^{1}I_{6}$, 393 nm).
We have investigated the process of quenching of fluorescence from the 3P0^{3}P_{0}3P0​ state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in La0.72{\mathrm{La}}_{0.72}La0.72​Pr0.25{\mathrm{Pr}}_{0.25}Pr0.25​Nd0.03{\mathrm{Nd}}_{0.03}Nd0.03​F3{\mathrm{F}}_{3}F3​ due to cross relaxation to Pr and Nd ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature in the (2-70)-K region. Cross relaxation occurs either directly or through a donor-donor transfer within the inhom-geneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from previous fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint according to models for fluorescence decay in the presence of traps. In general the decay is consistent with an electric dipole-dipole transfer mechanism. At 2 K the decay can be well described by a direct transfer to Pr and Nd traps without donor-donor transfer. The temperature dependence of the decay at long times can be described for 35<T<7035<T<7035<T<70 K by the hopping model. The agreement with theory is much better if the cross relaxation to Nd ions is assumed to occur mainly via the lowest Stark level of the 4I92^{4}I_{\frac{9}{2}}4I29​​ manifold.