1. Institute of Crystallography, Russian Academy of Sciences, Russia;2. Institute of Optics and Atomic Physics, Technical University of Berlin, Berlin, Germany;3. Department of Inorganic Chemistry, Faculty of Science, Charles University, Czech Republic;4. Institute for Laser Science, University of Electro‐Communications, Tokyo 182–8585, Japan;5. Section Crystallography, Institute of Geology and Mineralogy, University of Cologne, Germany;6. Section Crystallography, Institute of Geology and Mineralogy, University of Cologne, GermanyE‐mail:
Abstract:
The non‐centrosymmetric polar tetragonal (P 41) barium antimony tartrate trihydrate, Ba[Sb2((+)C4H2O6)2]·3H2O, was found to be an attractive novel semi‐organic crystal manifesting numerous χ (2)‐ and χ (3)‐nonlinear optical interactions. In particular, with picosecond single‐ and dual‐wavelength pumping SHG and THG via cascaded parametric four‐wave processes were observed. High‐order Stokes and anti‐Stokes lasing related to two SRS‐promoting vibration modes of the crystal, with ωSRS1 ≈ 575 cm?1 and ωSRS2 ≈ 2940 cm?1, takes place. Basing on a spontaneous Raman investigation an assignment of the two SRS‐active vibration modes is discussed.