Syntheses, crystal structures, and magnetic properties of two new organic-inorganic hybrid materials containing metal-bis(dithiolene) anion and substituted triphenylphosphinium

Abstract Two new organic-inorganic hybrid materials, [(Ph) 2 CHTPP][Ni(mnt) 2 ]( 1 ) and [(Ph) 2 CHTPP] 2 [Cu(mnt) 2 ]·2CH 3 CN( 2 ) (mnt = maleonitriledithilate, [(Ph) 2 CHTPP] +  = diphenylmethane-triphenylphosphinium), were prepared and characterized. Two compounds crystallize in the triclinic lattice with P -1 space group, and the adjoined anions form one-dimension chain structure through weak π⋯π or C⋯N interactions in 1 , and C H⋯S and C H⋯N hydrogen bonds through the solvent lattice acetonitrile molecule in 2 . The power X-ray diffraction patterns are in good agreement with the simulated patterns based on the crystal structures, indicating the purity of the as-grow crystals. FT-IR and UV–vis spectra were recorded and analyzed with the aid of the DFT calculation. The HOMO/SOMO and LUMO energy gaps were calculated by the DFT method explain charge transfer interactions take place within two materials. Thermal analysis shows two materials can be stable up to 171 °C for 1 and 215 °C for 2 . The variable-temperature susceptibility analysis shows that 1 is the para-magnetic system with a spin-gap at 110 K and 2 exhibits a weak antiferromagnetic exchange interaction as the temperature is lowered.