Molecule-based ferromagnets that exhibit strong second-harmonic genera
tion (SHG) are presented here for the first time. The strategy for pro
ducing such materials-replace the ''innocent'' bulky cations (C) in th
e C[M'M(ox)(3)] family of bimetallic magnets (M' is e.g. Mn and M = Cr
-III or Fe-III: the Figure shows the structure) by hyperpolarizable ca
tionic chromophores-is described and X-ray, magnetic, and SHG results
are reported.