Synthesis, growth, structural, thermal, optical properties of new metal-organic crystals: Methyltriphenylphosphonium iodide thiourea and methyltriphenylphosphonium iodide chloroform hemisolvate

• The title products were obtained by co-crystallization and slow evaporation.
• The compounds were characterized by single crystal, X-ray, FTIR, UV and DTA/TGA.
• Single crystal with optical of methyl-triphenylphosphonium iodidehas been obtained.
• SHG was observed from crystals of methyl-triphenylphosphonium iodide thiourea.

Crystals of methyltriphenylphosphonium iodide thiourea (1) and methyltriphenylphosphonium iodide chloroform hemisolvate (2) were obtained for the first time. Fourier transform infrared (FTIR) spectral studies have been performed to identify the functional groups. Thermogravimetric analysis (TGA) and differential thermal analysis (DTA) were used to study their thermal properties. The optical transmittance window and the lower cutoff wavelength have been identified by UV–vis studies. Crystals of the title compounds suitable for single crystal X-ray analyses were successfully grown by slow evaporation and diffraction data were collected to elucidate the molecular structure and interactions. The proton donors (phosphonium) and proton acceptor (iodine) in the structure of 1 provide infrastructure to introduce charge asymmetry while in 2 chloroform molecule is not involved in the charge transfer. An optical quality crystal of 1 (5×4×2 mm3) was obtained by macroseeding. The crystal has developed facets with major ones (001) and (00¯1). A crystal of 1 was tested with 1060 nm laser radiation and showed second harmonic generation (SHG).