2021, Alles, Adrian, Pan, Zhongben, Loiko, Pavel, Serres, Josep Maria, Slimi, Sami, Yingming, Shawuti, Tang, Kaiyang, Wang, Yicheng, Zhao, Yongguang, Dunina, Elena, Kornienko, Alexey, Camy, Patrice, Chen, Weidong, Wang, Li, Griebner, Uwe, Petrov, Valentin, Solé, Rosa Maria, Aguiló, Magdalena, Díaz, Francesc, Mateos, Xavier

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. 𝐼𝑎3¯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.

2022, Eremeev, Kirill, Loiko, Pavel, Braud, Alain, Camy, Patrice, Zhang, Jian, Xu, Xiaodong, Zhao, Yongguang, Liu, Peng, Balabanov, Stanislav, Dunina, Elena, Kornienko, Alexey, Fomicheva, Liudmila, Mateos, Xavier, Griebner, Uwe, Petrov, Valentin, Wang, Li, Chen, Weidong

We report on a detailed spectroscopic study of a Tm3+-doped transparent sesquioxide ceramic based on a solid-solution (lutetia – yttria, LuYO3) composition. The ceramic was fabricated using commercial oxide powders by hot isostatic pressing at 1600°C for 3 h at 190 MPa argon pressure. The most intense Raman peak in Tm:LuYO3 at 385.4 cm−1 takes an intermediate position between those for the parent compounds and is notably broadened (linewidth: 12.8 cm−1). The transition intensities of Tm3+ ions were calculated using the Judd-Ofelt theory; the intensity parameters are W2 = 2.537, W4 = 1.156 and W6 = 0.939 [1020 cm2]. For the 3F4 → 3H6 transition, the stimulated-emission cross-section amounts to 0.27 × 10−20 cm2 at 2059nm and the reabsorption-free luminescence lifetime is 3.47 ms (the 3F4 radiative lifetime is 3.85 ± 0.1 ms). The Tm3+ ions in the ceramic exhibit long-wave multiphonon-assisted emission extending up to at least 2.35 µm; a phonon sideband at 2.23 µm is observed and explained by coupling between electronic transitions and the dominant Raman mode of the sesquioxides. Low temperature (12 K) spectroscopy reveals a significant inhomogeneous spectral broadening confirming formation of a substitutional solid-solution. The mixed ceramic is promising for ultrashort pulse generation at >2 µm.