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Journal of Applied Physics

Nonequilibrium population distribution in excited electronic states of Tb3+ in Y3Al5O12

John B. Gruber, Dhiraj Kumar Sardar, Kelly L. Nash, Uygun V. Valiev, Vladimir Yu. Sokolov, Sharof A. Rakhimov

Published May 15, 2008• 4 citations
Publisher

Abstract

The Zeeman effect has been studied within the “green” range of luminescence due to the radiative 4f→4f transitions D54→F75 for the rare earth ion Tb3+ in yttrium aluminum garnet (Y3Al5O12) at a sample temperature of 85 K. The special features associated with the magnetic field dependence of the Zeeman splitting have been explained for transitions observed in the geometry of the longitudinal and transverse Zeeman effect. An analysis of the results obtained from the magneto-optical data indicates that in a magnetic field a nonequilibrium population distribution occurs between the sublevels of the quasidoublet state (Γ1,Γ4) in the D54 manifold. The energy of the quasidoublet state is approximately 20 585 cm−1.

DOI
10.1063/1.2921836

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The Zeeman effect has been studied within the “green” range of luminescence due to the radiative 4f→4f transitions D54→F75 for the rare earth ion Tb3+ in yttrium aluminum garnet (Y3Al5O12) at a sample temperature of 85 K. The special features associated with the magnetic field dependence of the Zeeman splitting have been explained for transitions observed in the geometry of the longitudinal and transverse Zeeman effect. An analysis of the results obtained from the magneto-optical data indicates that in a magnetic field a nonequilibrium population distribution occurs between the sublevels of the quasidoublet state (Γ1,Γ4) in the D54 manifold. The energy of the quasidoublet state is approximately 20 585 cm−1.
The spectra of luminescence and magnetic circular polarization of luminescence in the 1 D 2 → 3 F 4 emission band in thulium:yttrium-aluminum garnet Tm3+:YAG (Tm3+:Y3Al5O12) have been investigated at temperatures T = 78 and 293 K, respectively. Based on the analysis of the magnetooptical and optical spectra, the optical transitions between the Stark sublevels of the 3 F 4 and 1 D 2 multiplets in Tm3+:YAG were identified. It is shown that the symmetry and energies of the Stark sublevels of the 3 F 4, 1 D 2, and 3 H 6 multiplets, found experimentally from magnetic and magnetooptical studies, confirm the results of theoretical calculations of the energy spectrum of the rare earth Tm3+ ion in YAG.
An investigation was made of the absorption spectrum of Cr 3+ ions in the ground ( 4 A 2 ) and metastable ( 2 E) states, and of the luminescence spectrum of the same ions in Y 3 Al 5 O 12 crystals at 300 and 77°K. The effective absorption cross sections were determined for the 4 A 2 state. The luminescence deexcitation time was found to be 1.5 and 9 msec at 300 and 77°K, respectively. The absorption spectrum of the 2 E state had four wide absorption bands with maxima at 16,700, 23,300, 28,600, and 40,500 cm –1 . The theoretical energy level scheme of Cr 3+ was calculated for Dq = 1725 cm –1 , G = 640 cm –1 , C = 3200 cm –1 , v = 495 cm –1 , and v' = 259 cm –1 , making an allowance for the mixing of the Γ trig S states. The experimentally observed absorption bands were attributed to specific transitions and the theoretical and experimental intensities were compared.
Broad bandwidth 5d→4f transitions in Ce3+ have been considered for tunable laser action. In this letter, optical probe measurements of excited Ce3+ ions in Y3Al5O12 show that stimulated emission in the 550–610-nm region is not possible at 295 K because of excited-state absorption. Transient measurements demonstrate that part of this loss has ≈75-ns lifetime and is associated with absorption from the lowest 5d level; a longer-lifetime loss is also observed. The excited-state-absorption loss is reduced at lower temperatures.
Resonantly enhanced, near-ultraviolet 4f3 → 4f25d two-photon transitions have been observed in trivalent neodymium-doped yttrium aluminum garnet (Nd3+:Y3Al5O12). The two-photon excitation spectra over the 40 400–46 730 cm−1 transition energy range are characterized by sharp resonance peaks on a slowly varying background caused by nonresonant transitions. The peak two-photon cross section involving the 2P1/2 resonant intermediate state is 9 × 10−51 cm4 s, and the integrated cross section is 2.2 × 10−38 cm4.
The creation of well-understood structures using spectral hole burning is an important task in the use of technologies based on rare-earth ion-doped crystals. We apply a series of different techniques to model and improve the frequency dependent population change in the atomic level structure of thulium yttrium gallium garnet (Tm:YGG). In particular we demonstrate that, at zero applied magnetic field, numerical solutions to frequency-dependent three-level rate equations show good agreement with spectral hole-burning results. This allows us to predict spectral structures given a specific hole-burning sequence, the underpinning spectroscopic material properties, and the relevant laser parameters. This enables us to largely eliminate power-dependent hole broadening through the use of adiabatic hole-burning pulses. Although this system of rate equations shows good agreement at zero field, the addition of a magnetic field results in unexpected spectral diffusion proportional to the induced Tm ion magnetic-dipole moment and average magnetic-field strength, which, through the quadratic Zeeman effect, dominates the optical spectrum over long timescales. Our results allow optimization of the preparation process for spectral structures in a large variety of rare-earth ion-doped materials for quantum memories and other applications.