Using (N-vinylcarbazole)Cr(CO)₃ complex as template substrate, a novel organometallic complex with nonplanar intramolecular charge transfer property was synthesized by replacing a CO group with cationic allyl ligand. The composition and structure of the title complex were characterized by elemental analysis, IR, ¹H and ¹³C NMR spectra. Electronic absorption and photoluminescence studies suggested that ligand exchange on the organometallic moiety offered control of the photophysical properties for this class of materials. Third-order nonlinear optical properties of the complexes and ligands in this work were measured with forward degenerate four-wave mixing (DFWM) method and discussed in relation to the metal coordination and ligand replacement.

Key words: charger transfer, photophysical, ionic complex