We report on UV-pumping of a visible Tb:LiLuF4 laser emitting at 544 and 588 nm. Pumping with a frequency-doubled Ti:sapphire laser at 359 nm significantly improves the absorption efficiency compared to conventional in-band pumping at ~488 nm and cross relaxation from the excited level 5D3 efficiently populates the upper laser level 5D4. In this way, optical efficiencies of 29% and 12%, respectively, are obtained with respect to the incident pump power. A passively Q-switched Tb:LiLuF4 laser at 544 nm using a Co2+-doped MgAl2O4 as a saturable absorber yields 23-µJ pulses at 3.5 kHz with a pulse duration of ~200 ns.
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