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Organic dye molecules have been widely used in solution as amplifying media in tunable lasers. The possibility of trapping these molecules in a solid state matrix may lead to a new field of application outside the laboratory. Many types of matrices can be used. We present results with new hybrid organic/inorganic xerogels prepared by hydrolysis-condensation of the methyl- or vinyl-triethoxysilane precursor under acid-catalyzed hydrolysis and basic-catalyzed condensation. Organic methyl or vinyl groups attached to the silica network provide a favorable environment to dye fluorescence. We have studied the effect induced by using different basic catalysts: N-(2-aminoethyl)-3-aminopropyltrimethoxysilane and 3- aminopropyltriethoxysilane are found to lead to the best matrix characteristics. Perylenes and pyrromethenes were chosen because of their thermal- and photo-stability. After gelation, 10 mm thick samples, polished to a surface roughness of about 4 nm, are placed in a plano- concave cavity as gain media and pumped by a frequency doubled nanosecond Q:switched Nd:YAG laser. Efficiency is the greatest with a pyrromethene 597 doped sample: more than 6 mJ output energy for a 10 mJ pump energy (2 J/cm2 fluence) leading to a slope efficiency of 63%. The lifetime of the laser emission when the same point of the sample is sequentially used is also an important characteristic. Best results are obtained with perylene red dye: for a pump energy of 0.7 mJ at 1 Hz repetition rate, the output energy is still 50% of the initial value (0.1 mJ) after 80,000 shots. For a pyrromethene 597 doped MTEOS sample, it appears that the measured lifetimes are independent of the operating frequency in the 0.2 - 20 Hz range, indicating a reasonable heat conductivity for this type of matrix. We have also studied tunability by adding a grating or prism to the cavity: a typical tunability of over 50 nm or more is obtained with many of these dyes. Finally we report laser activity obtained with rhodamine B doped xerogels in which the dye molecules were covalently bonded to the silica network in order to stabilize the organic molecule structure.
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