A novel eta(6)-complex of N-allylcarbazole containing chromium tricarbonyl was synthesized. This complex was hydrosilylated with polymethylhydrosiloxane to afford a substituted polymer. Both the complex and the polymer were characterized by classical spectroscopy techniques (FTIR, NMR, and UV-vis), gel permeation chromatography, elemental analysis, and thermal analysis (TGA and DSC). The glass transition temperature of the polymer was found to be above 100 degrees C and its thermal decomposition temperature was above 280 degrees C. The polymer was amorphous in nature and formed excellent homogeneous films of good optical transparency. The third nonlinear optical properties of this polymer film coated on quartz substrate were studied by time-resolved forward degenerate four-wave mixing (DFWM). (c) 2007 Wiley Periodicals, Inc.