Chiral effects in the second‐order optical nonlinearity of a poly(isocyanide) monolayer**

The influence of chirality on the nonlinear optical properties of poly(isocyanide)s is examined. It is found that the chiral and nonlinear properties can occur on different levels of the molecular structure and can therefore be separately tuned, but that they still can be coupled together. The NLO properties of chiral molecules can also be enhanced significantly byoptimizing the magnetic contriutions to the nonlinearity, an important result for applicatons in electro‐optics.