Communication: The influence of chirality on the nonlinear optical pro
perties of poly(isocyanide)s is examined. It is found that the chiral
and nonlinear properties can occur on different levels of the molecula
r structure and can therefore be separately tuned, but that they still
can be coupled together. The NLO properties of chiral molecules can a
lso be enhanced significantly by optimizing the magnetic contributions
to the nonlinearity, an important result for applications in electro-
optics.