The third-order nonlinear optical susceptibility chi(3)(-3omega;omega,
omega,omega) of propylmethylpolyazine thin films as measured by the th
ird harmonic generation is reported. The chi(3)(-3omega;omega,omega,om
ega) values of propylmethylpolyazine that possess statistically altern
ating methyl and propyl substituents on the carbon atoms along the con
jugated chain were found to be 8.0X10(-12) esu off resonance at 1.5 mu
m fundamental radiation. The interesting third-order nonlinear propert
ies presumably originate from the unique periodicity of the main pi-el
ectron-conjugated polyazine backbone.