Multisite optical spectra and energy levels of trivalent thulium ions in yttrium scandium gallium garnet

Abstract

Intrinsic structural disorder in scandium-substituted garnets, attributed to mixed occupancy of certain sites in the crystal lattice by different cations, has direct consequences for the optical spectra of rare-earth activator ions dispersed over multiple sites. In trivalent thulium-doped yttrium scandium gallium garnet (Tm3+:YSGG), site-selective laser excitation spectra reveal the presence of Tm3+ ions in regular D2 sites, disturbed regular sites, and in octahedral C3i sites. Absorption spectra obtained at 4 K between 0.26 and 1.85 μm are broader than those observed in more-ordered crystal hosts and include structure attributed to Tm3+ ions in sites of other than D2 symmetry. A crystal-field splitting calculation was carried out in which a parametrized Hamiltonian (including Coulombic, spin-orbit, and crystal-field terms for Tm3+ ions in D2 symmetry) was diagonalized for all manifolds of the Tm3+ (4f12) configuration. The rms deviation between 52 experimental and calculated Stark levels of Tm3+ in regular D2 sites was 5 cm−1.