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A series of high quality x%Pr3+:BaF2 (x = 0.6, 1, 2); (1%Pr3+, 2%Na+):BaF2; (1%Pr3+, y%Ca2+):BaF2 (y = 3, 5) and (0.6%Pr3+, 10%R3+):BaF2 (R = Y, Lu, Gd) crystals were grown by temperature gradient technique (TGT). The Raman spectra, absorption spectra, fluorescence spectra, and fluorescence decay lifetime were measured. XRD patterns indicate that the as-synthesized samples are pure BaF2 phase. The absorption cross-section of Pr3+ ions in the BaF2 matrix can be greatly improved by co-doping R3+ ions, while improvement by Na+ and Ca2+ ions is marginal. The fluorescence characteristic of Pr3+ ions can be effectively regulated by co-doping Na+, Ca2+, R3+ (R = Y, Lu, Gd) ions of different valence states. When R3+ ions are introduced, the fluorescence spectra show the strongest orange emission and the CIE chromaticity coordinates of Pr3+ ions are also in the orange region. When single-doped Pr3+ ions and Na+ or Ca2+ ions are introduced, the fluorescence lifetime of the 3P0 level is double exponential decay, and the short lifetime is the main proportion. However, the fluorescence centers tend to homogeneous and stable by R3+ ions co-doping and the fluorescence lifetime exhibits single-exponential decay, which is fitted to 49.7 μs, 47.8 μs and 49.6 μs of (0.6%Pr3+, 10%R3+):BaF2 (R = Y, Lu, Gd), respectively. All the results show that (Pr3+, Gd3+):BaF2 and (Pr3+, Na+):BaF2 are excellent laser gain media for high-efficiency orange and red laser operation. [ABSTRACT FROM AUTHOR]