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Two kinds of new Ormosil xerogels derived from GPTMS (3-glycidyl propyl trimethoxisilane) and TEOS (tetraethoxysilane) or GPTMS and Ti(OBu)4 (tetrabutoxytitanate) were synthesized via the sol-gel method as dye laser host. Their optical properties, microstructure characteristics and surface laser damage thresholds have been reported. The effects of dye matrix combination on the fluorescence emission, slope efficiency, photostability and tunable bandwidth were examined. Laser oscillation was easily achieved near 620 nm with a slope efficiency of 29% from DCM doped SiO2-Ormosil pumped by a frequency-doubled radiation from a Q-switched Nd:YAG laser. The laser wavelength was tunable over 59nm, and the laser output energy had only a 10% reduction after 2.5×104 pulses at a pump repetition rate of 1 Hz and a pump intensity of 1 J/cm2.

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