Large single crystals of polar tetragonal thallium antimony(III) tartrate dihydrate, Tl(2)[Sb2((+)C4H2O6)2].2H2O, are grown. The crystal structure (s.g.
P41), which contains the binuclear complex group [Sb2(C4H2O6)2](2-) and dimer groups [Tl2O8(H2O)2], is given, together with vibrational spectra, refractive indices and their dispersion, and an analysis of SHG phase matching possibility and SHG powder measurements. The crystals allow type I phase matching for laser wavelengths >= 1.0103 µm.
In addition, a new monoclinic (s.g. C2) antimony(III) tartrate of composition Mg[Sb3((+)C4H2O6)2((+)C4H4O6)((+)C4H5O6)].11H2O and its crystal structure, which contains a novel type of antimony tartrate complex group [Sb3(C4H2O6)2(C4H4O6)(C4H5O6)], is presented.