This study successfully grew Yb3+-doped Y2Mg3-xCax(SiO4)3 (x = 0, 0.125, 0.25, 0.375, 0.5, 0.625, 0.75) (Yb: YCMS) novel single crystals with multiple disordered structures. To the best of our knowledge, this is the first systematic report on the relationship between the luminescence properties (including emission intensity, emission peak position, full width half maximum, and fluorescence lifetime) and the local structure of the luminescent ions based on first-principles calculations. The wide half-height width of emission (103.10 nm@1047 nm) have been realized on the first-grown Yb: YCMS crystals. This study provides a novel solution for designing laser crystals with tunable optical properties. The comprehensive properties of Yb3+-doped YCMS crystals, such as ultra-wide emission bandwidth and high fluorescence lifetime, are promising gain materials for ultrafast laser applications.
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