Trigonal Na3Li(MoO4)2·6H2O - a new many-phonon SRS molybdate crystal offering numerous nonlinear-laser interactions: several cascaded lasing (χ(3)↔χ(2)) effects and more than sesqui-octave Stokes and anti-Stokes comb generation under one-micron picosecond pumping

Trigonal Na3Li(MoO4)2·6H2O was found to be an attractive, simultaneously χ(2)‐ and χ(3)‐active nonlinear optical crystal. We investigated its basic optical properties and observed several nonlinear effects, namely many‐phonon SRS, almost twooctave Stokes and anti‐Stokes lasing combs, SHG, THG, and efficient cascaded (χ(3)↔χ(2))‐generation, as well as SRS arising from nonlinear interaction of two different χ(3)‐active vibrations. All recorded nonlinear‐lasing components were identified and attributed to SRS‐promoting vibration modes. A short review of nonlinear‐laser molybdates is given. (© 2009 by Astro Ltd., Published exclusively by WILEY‐VCH Verlag GmbH & Co. KGaA)