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In this paper, the Floating zone technique was used to grow high-quality Cr3+:YScO 3 crystals. The absorption cross-sections of the 4A 2 →4T 1 transition and 4A 2 →4T 2 transitions were calculated to be 1.71 × 10−20 cm2 at 488 nm and 0.72 × 10−20 cm2 at 666 nm, respectively. The crystal field strength Dq, Racah parameters B, and C were calculated to be 1502 cm−1, 533 cm−1, and 3362 cm−1, respectively. In the Cr3+:YScO 3 crystal, the effective phonon energy and Huang-Rhys factor S were calculated to be 284 cm−1 and 8.62, respectively. The emission cross-section at 988 nm corresponding to the 4T 2 →4A 2 transition was calculated to be 1.44 × 10−20 cm2 with full width at half maximum (FWHM) of 318 nm. All the results show that Cr3+:YScO 3 crystal has the potential to be a tunable and ultrafast laser crystal. • Cr:YScO 3 crystals were successfully grown by the Floating zone technique(FZ) method. • Broad emission spectrum with full width at half maximum (FWHM) of 318 nm in Cr:YScO 3 crystals was observed. • Spectral properties and crystal field parameters of Cr:YScO 3 crystals were investigated and analysed. [ABSTRACT FROM AUTHOR]