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Spectroscopy of solid-solution transparent sesquioxide laser ceramic Tm:LuYO3

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.