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Quantum Electronics

Up-conversion and excitation energy transfer between impurity ions in Pr3+: Y2SiO5, Pr3+: Lu2SiO5, and Pr3+: Gd2SiO5crystals

Nikolay V Znamenskiy, Eduard A. Manykin, Yurii V Orlov, Evgenii A Petrenko, T. G. Yukina, Yu. V. Malyukin, P.N. Zhmurin, Alexander N. Lebedenko, A. A. Masalov

Published Jul 31, 2004• 4 citations
Publisher

Abstract

Anti-Stokes fluorescence from the 3 P 0 level of impurity ions was detected in Pr 3+ : Y 2 SiO 5 , Pr 3+ : Lu 2 SiO 5 , and Pr 3+ : Gd 2 SiO 5 crystals non-resonantly pumped by laser radiation with a certain power density. The integrated intensity of the anti-Stokes fluorescence depends nonlinearly on the pump power density. As the atomic concentration of impurity ions was increased from 0.3% to 0.6% and 1.8%, the anti-Stokes fluorescence intensity was saturated due to the concentration quenching of the 1 D 2 term of the impurity Pr 3+ ions. The anti-Stokes fluorescence and quenching of the 1 D 2 term occur due to the cross relaxation of the electronic energy of excited terms of the Pr 3+ ions.

DOI
10.1070/qe2004v034n07abeh002812

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Anti-Stokes fluorescence from the 3 P 0 level of impurity ions was detected in Pr 3+ : Y 2 SiO 5 , Pr 3+ : Lu 2 SiO 5 , and Pr 3+ : Gd 2 SiO 5 crystals non-resonantly pumped by laser radiation with a certain power density. The integrated intensity of the anti-Stokes fluorescence depends nonlinearly on the pump power density. As the atomic concentration of impurity ions was increased from 0.3% to 0.6% and 1.8%, the anti-Stokes fluorescence intensity was saturated due to the concentration quenching of the 1 D 2 term of the impurity Pr 3+ ions. The anti-Stokes fluorescence and quenching of the 1 D 2 term occur due to the cross relaxation of the electronic energy of excited terms of the Pr 3+ ions.
In the Pr3+ -doped Y2SiO5, the population in 1D2 of Pr3+ can be transferred to 3P0 state via non-radiative energy transfer by the laser excitation in resonance with 3H4-->1D2 , and we can experimentally study the Stark splitting of 3H4 energy level via 3P0 -->3H4 anti-Stokes emission spectra. Because the anti-Stokes emission spectra can avoid the energy transfer between different crystallographic site 1D2 energy levels, the above splitting lines attribution is more accurate than the assignment via 1D2-->3H4 Stokes spectra by the laser excitation in resonance with 3H4-->1D2. In addition, the character of the anti-Stokes fluorescence decay time was observed.
In the Pr(superscript 3+) -doped Y2SiO5, the population in 1D2 of Pr(superscript 3+) can be transferred to 3P0 state via non-radiative energy transfer by the laser excitation in resonance with 3H4→1D2, and we can experimentally study the Stark splitting of 3H4 energy level via 3P0→3H4 anti-Stokes emission spectra. Because the anti-Stokes emission spectra can avoid the energy transfer between different crystallographic site 1D2 energy levels, the above splitting lines attribution is more accurate than the assignment via 1D2→3H4 Stokes spectra by the laser excitation in resonance with 3H4. In addition, the character of the anti-Stokes fluorescence decay time was observed.
In a Y2SiO5:Pr3+ crystal characterized by two non-equivalent Pr3+ optical centers, the interaction mechanisms between Pr3+ ions as well as between Pr3+ ions and a crystal lattice have been studied. It has been shown that along with the electron-phonon interaction, the interaction between Pr3+ ions and two-level systems made an additional contribution to the homogeneous linewidth of the 3H4↔3P0 optical transition. Two different mechanisms of the Pr3+ interionic coupling have been found. The first mechanism is associated with a dipole-dipole interaction between non-equivalent Pr3+ optical centers, while the other one is governed by a cooperative cross relaxation of the excitation energy among the same type Pr3+ optical centers.
We have investigated the process of quenching of fluorescence from the 3P0^{3}P_{0}3P0​ excited state of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ due to cross relaxation among the Pr ions. The fluorescence decay of the ensemble of Pr ions after pulsed excitation is measured as a function of temperature for Pr concentration of 20 mol%. About 12% of the ions are in nonquenching sites and contribute an exponential component to the decay. The remainder of the decay originates from the bulk of the ions in quenching sites. Cross relaxation occurs directly in steps after transfer within the inhomogeneous line. Knowledge of the dynamics occurring within the inhomogeneous line derived from fluorescence line-narrowing experiments is used to analyze the cross-relaxation process from a microscopic viewpoint based on a recent model for fluorescence in the presence of traps. At 2 K the decay is consistent with an electric dipole-dipole transfer mechanism with a nearest-neighbor quenching rate of 8.9 \ifmmode\times\else\texttimes\fi{} 104{10}^{4}104 ${\mathrm{s}}^{\ensuremath{-}1}$ which is independent of temperature for T<32T<32T<32 K and which successfully predicts the observed decay rate in PrF3{\mathrm{F}}_{3}F3​. The temperature dependence of the decay for $8\ensuremath{\le}T\ensuremath{\le}32$ K is well described by a hopping model for excitation trapping. For T>35T>35T>35 K an activation process becomes dominant consistent with the onset of cross relaxation involving the 1D2(5)^{1}D_{2}(5)1D2​(5) and 3H6(1)^{3}H_{6}(1)3H6​(1) states in which a 190-${\mathrm{cm}}^{\ensuremath{-}1}$ phonon is created.
We consider a theoretical model for laser cooling with anti-Stokes fluorescence of a Yb3+:YAG sample. We have estimated the fluorescence power density removed from the system with spontaneous emission, the power density radiated with stimulated emission as well as the heat power density generated in the system by non-radiative decays from the impurities in the host material. We have investigated the influence of each of these power densities on the cooling process in Yb3+:YAG system. It has been shown how the temperature dependences of the different parameters of the system as well as the concentration of the impurities in the host influence the final temperature of the cooled sample.
This paper shows that the satellite lines that appear in the absorption and fluorescence spectra of neodymium ions in a LaF3 crystal at concentrations of about 0.5 at.% and the accompanying lines of the isolated ion are caused by pairwise interaction of the Nd3+ ions. Double optical resonance is used to study the structure of the satellite lines in the neighborhood of the 4I9/2→4G5/2 transition of the isolated ion (wavelength 5777.1 Å), hidden by inhomogeneous broadening. When neodymium ion pairs are excited by resonance laser radiation, the presence of anti-Stokes components is recorded in the fluorescence spectrum (up-conversion). It is shown that the main up-conversion mechanism is cumulative pair excitation. These results are convincing evidence that the suppression of absorption from excited levels can be experimentally observed in condensed media.