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We report the successful development of an all-solid state laser based on a Czochralski method-grown cerium-doped lithium calcium aluminum fluoride (Ce3+:LiCaAlF6) crystal as the gain medium. Results for the broadband, narrow linewidth and short pulse laser emission are obtained by pumping with 7 ns pulses at 266 nm from the fourth harmonics of a Nd:YAG laser operating at 10 Hz repetition rate. The effects of output coupler reflectivitiy, resonator length and pump energy on the laser pulse duration were explored. With broadband configuration, a maximum output pulse energy of a few mJ was achieved. Sub-nanosecond UV laser pulses were generated from a low-Q and short resonator under near threshold pump energy. By replacing the end mirror with a grating, tunability from 281 nm to 299 nm with linewidth of about 0.2 nm is achieved. For high power ultrashort ultraviolet laser development, we have investigated the prospects of using a diamond-cut Ce:LiCAF crystal in a two-side-pumping configuration, and performed calculations on the optimum geometry, size, and absorption coefficient that will serve as a guideline when developing a UV laser oscillator and femtosecond amplifier. Results show that there is a trade-off between homogeneity and absorption ratio for absorption coefficients greater than 1.5 cm−1. Moreover, a larger crystal with lower doping concentration would be more homogeneous and would have a higher absorption ratio, regardless of geometry. Our results suggest the possibility of developing an all-solid-state ultraviolet laser operating at TW level by appropriately designing the amplifier crystal in conjunction with a multiple-beam side-pumping configuration.