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The spectral properties of lightly doped Er:CaF 2 and Er,Pr:CaF 2 single crystals were investigated. Benefited from particular clustering effect, 2.79 μm continuous-wave (CW) laser operation was demonstrated in lightly doped 3 at.% Er:CaF 2 crystal. After co-doping small amount of Pr 3+ , the lifetime gap between Er 3+ : 4 I 11/2 and Er 3+ : 4 I 13/2 was shortened from 7.86 ms to about 1 ms. Moreover, the near-infrared and up-conversion fluorescence were significantly quenched. Thus, the CW laser performance was greatly improved. The slope efficiency was effectively improved from 8.0% to 15.8%. [ABSTRACT FROM AUTHOR]

• A series of 0.6 at% Pr:CaF 2 -RF 3 (R= Y3+, Gd3+, Lu3+) crystals were successfully grown by the temperature gradient technique(TGT) method. • By co-doping R3+ ion (R=Y3+, Gd3+, Lu3+), the spectral performance of the crystals could be significantly improved and the function effect is also different. • The spectral performance and spectral quality factor of the crystals were systematically described and compared for the first time. • The spectral modulation effect caused by Y3+, Gd3+ and Lu3+ co-doping ion was discussed. A series of 0.6 at% Pr:CaF 2 -RF 3 (R = Y3+, Gd3+, Lu3+) crystals have been successfully grown by the temperature gradient technique(TGT). The absorption spectra, fluorescence spectra, and fluorescence decay curves were measured and analyzed at room temperature. When the R3+ concentration is higher than a certain value, the diffraction peaks of Pr:CaF 2 -RF 3 crystals were well indexed to the (Ca,Y)F 2 phase. By co-doping R3+ ion (R=Y3+, Gd3+, Lu3+), the spectral performance of the crystals could be significantly improved and the function effect is also different. For 0.6 at% Pr, 28.5 at% Y:CaF 2 crystal, the fluorescence lifetime of 3P 0 energy level was fitted to be 45.46 µs, and the emission cross sections of 3P 0 →3H 6 (605 nm), and 3P 0 →3F 2 (641 nm) were calculated to be 1.78 × 10−20 cm2, and 4.61 × 10−20 cm2 with the full width at half (FWHM) of 20.1 nm and 6.8 nm, respectively. The 0.6 at% Pr, 28.5 at% Y:CaF 2 crystal could be favorble laser medium for ultra-fast laser opreration at 605 nm and 641 nm. For 0.6 at% Pr, 18 at% Gd:CaF 2 and 0.6 at% Pr, 10 at% Lu:CaF 2 crystals, the spectral quality factors σ em• τ f of 3P 0 →3F 2 transition (642 nm) were calculated to be 614.18 × 10−20 cm2•µs and 506.36 × 10−20 cm2•µs with the FWHM of 3.7 nm and 5.3 nm. All the results show that 0.6 at% Pr, 18 at% Gd:CaF 2 and 0.6 at% Pr, 10 at% Lu:CaF 2 crystals are promising gain media for high-efficiency visible laser output at 642 nm, which would compete with commercial Pr: YLF crystal in the future. [ABSTRACT FROM AUTHOR]