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2-Amino-4-nitroaniline crystallizes in a noncentrosymmetric space group giving it significant potential for second-order nonlinear optical properties (NLO) in the bulk. The theoretically predicted NLO properties at the molecular level are confirmed using various methods like X-ray diffraction, conventional and polarized IR spectroscopy, thermal and elemental analysis.

The structures of the [{Os(PPh3)2(pap)}2(ca)](CIO4)2, [Os(PPh3)2(pap)(ca)], and [{Os(PPh3)2(CO)2}2(r-ca)] complexes are determined by X-ray crystallography. In the [{Os(bpy)2}(ca)](super 2+) and [{Os(PPh3)2(pap)2(ca)](super 2+) complexes, the chloranilate dianion is serving as a tetradentate bridging ligand.

The crystal structure and optical and magnetic properties of the newly synthesized 4-cyanopyridinium hydrogensquarate monohydrate are analyzed by using single-crystal X-ray diffraction and other spectroscopic methods. The unusual red color of the compound in the solid state is shown to be due to a strong bathochromic shift of the charge transfer band within the stable layers formed by the (2HSq.2[H.sub.2]O) fragments.