Spectra, energy levels, and symmetry assignments for Stark components of Eu3+(4f6) in gadolinium gallium garnet (Gd3Ga5O12)

Absorption and fluorescence spectra observed between 450 and 750 nm at 85 K and room temperature (300 K) are reported for Eu3+(4f(6)) in single-crystal Czochralski-grown garnet, Gd3Ga5O12 (GGG). The spectra represent transitions between the L-2S+1(J) multiplets of the 4f(6) electronic configuration of Eu3+ split by the crystal field of the garnet. In absorption, Eu3+ transitions are observed from the ground state, F-7(0). and the first excited multiplet, F-7(1), to multiplet manifolds D-5(0), D-5(1), and D-5(2). The Stark splitting of the F-7(J) multiplets (J=0-6) was determined by analyzing the fluorescence transitions from D-5(0), D-5(1), and D-5(2) to F-7(J). The Eu3+ ions replace Gd3+ ions in sites of D-2 symmetry in the lattice during crystal growth. Associated with each multiplet manifold are 2J+1 non-degenerate Stark levels characterized by one of four possible irreducible representations (irreps) assigned by an algorithm based on the selection rules for electric-dipole (ED) and magnetic-dipole (MD) transitions between Stark levels in D-2 symmetry. The quasi-doublet in D-5(1) was characterized by an analysis of the magneto-optical spectra obtained from the transitions observed between D-5(1) and F-7(1). A parameterized Hamiltonian defined to operate within the entire 4f(6) electronic configuration of Eu3+ was used to model the experimental Stark levels and their irreps. The crystal-field parameters were determined through use of a Monte-Carlo method in which nine independent crystal-field parameters, B-q(k), were given random starting values and optimized using standard least-squares fitting between calculated and experimental levels. The final fitting standard deviation between 57 calculated-to-experimental Stark levels is 5.9 cm(-1). The choice of coordinate system, in which the nine B-q(k) are real and the crystal-field z-axis is parallel to the [0 0 1] crystal axis and perpendicular to the xy plane, is identical to the choice we used previously in analyzing the spectra of Er3+ and Ho3+ garnets. (C) 2011 Elsevier B.V. All rights reserved.