RESUMEN
The reaction of CoCl2 with the naphthalene methylated triphenylphosphinium bromide [n-NAPMeTPP]Br (n=1, 2) and KSCN, in a methanolic medium at ambient temperature, leads to the self-assembly formation of hybrid 2:1 organic-inorganic molecular solids, [1-NAPMeTPP]2[Co(NCS)4](1) and [2-NAPMeTPP]2[Co(NCS)4](2) ([NAPMeTPP](+)=(naphthylmethylene)(triphenyl)phosphinium), which have been characterized by elemental analyses, IR spectroscopy, UV-Vis spectra, ESI-MS, molar conductivity and single-crystal X-ray diffraction structural analyses. Compound 1 crystallizes in the orthorhombic space group Pna21, while 2 does in the monoclinic space group C2/c. The cations form a dimer through the weak intermolecular C-Hâ¯π interactions in 1 and πâ¯π interaction in 2, while the anion and cation are linked by the C-Hâ¯S hydrogen bond in 1. Two molecular solids show dual functionalities: (1) the broad fluorescence emission around 400nm in the solid state at room temperature; (2) the weak antiferromagnetic coupling behavior.