Tm³⁺-doped calcium lithium tantalum gallium garnet (Tm:CLTGG): novel laser crystal

Abstract

We report on the development of a novel laser crystal with broadband emission properties at ∼2 µm – a Tm3+,Li+-codoped calcium tantalum gallium garnet (Tm:CLTGG). The crystal is grown by the Czochralski method. Its structure (cubic, sp. gr. I a 3 ¯ d , a = 12.5158(0) Å) is refined by the Rietveld method. Tm:CLTGG exhibits a relatively high thermal conductivity of 4.33 Wm-1K-1. Raman spectroscopy confirms a weak concentration of vacancies due to the charge compensation provided by Li+ codoping. The transition probabilities of Tm3+ ions are determined using the modified Judd-Ofelt theory yielding the intensity parameters Ω2 = 5.185, Ω4 = 0.650, Ω6 = 1.068 [10−20 cm2] and α = 0.171 [10−4 cm]. The crystal-field splitting of the Tm3+ multiplets is revealed at 10 K. The first diode-pumped Tm:CLTGG laser generates 1.08 W at ∼2 µm with a slope efficiency of 23.8%. The Tm3+ ions in CLTGG exhibit significant inhomogeneous spectral broadening due to the structure disorder (a random distribution of Ta5+ and Ga3+ cations over octahedral and tetrahedral lattice sites) leading to smooth and broad gain profiles (bandwidth: 130 nm) extending well above 2 µm and rendering Tm:CLTGG suitable for femtosecond pulse generation.