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Subject: Solid solutions ×

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    Spectroscopy of solid-solution transparent sesquioxide laser ceramic Tm:LuYO3
    (Washington, DC : OSA, 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.
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    Dimethyl carbonate synthesis from carbon dioxide using ceria–zirconia catalysts prepared using a templating method: characterization, parametric optimization and chemical equilibrium modeling
    (London : RSC Publishing, 2016) Kumar, Praveen; With, Patrick; Srivastava, Vimal Chandra; Shukla, Kartikeya; Gläser, Roger; Mishra, Indra Mani
    In this paper, a series of CexZr1−xO2 solid solution spheres were synthesized by exo- and endo-templating methods and tested for dimethyl carbonate (DMC) synthesis using direct conversion of CO2. The synthesized catalysts were characterized by X-ray diffraction (XRD), N2-physisorption, scanning electron microscopy (SEM), and CO2/NH3-temperature-programmed desorption (TPD). Formation of CexZr1−xO2 solid solutions with tetragonal and cubic crystal structures depending on cerium/zirconium compositions was confirmed by XRD analysis. The specific surface area of the mixed oxide decreased and the average pore diameter increased with an increase in the ceria content, with the exception of the mixed oxides with x = 0.4–0.5 i.e. Ce0.4Zr0.6O2 and Ce0.5Zr0.5O2. The basic and acidic site density of the synthesized catalysts was in the order: ZrO2 < CeO2 < Ce0.5Zr0.5O2, and the basic and acidic site density per unit area followed the same order. The best Ce0.5Zr0.5O2 catalyst was further used for the optimization of reaction conditions such as reaction time, reaction temperature, catalyst dose and reusability for DMC synthesis. Furthermore, study of chemical equilibrium modeling was done using the Peng–Robinson–Stryjek–Vera equation of state (PRSV-EoS) along with the van der Waals one-fluid reaction condition so as to calculate change of Gibbs free energy (ΔG°) and heat of reaction (ΔH°).