Abstract: Two new phosphonate-terminated polar azo dyes, one that is substantially rigid (1) and the other with a large molecular hyperpolarizability (2), were designed and incorporated into zirconium-based surface multilayers. Second harmonic generation (SHG) was observed from the multilayers as a function of incident and polarization angles and compared with that from the previously reported aminophenylazophenylphosphonic acid chromophore 3. The ...