Second order nonlinear optical properties (NLO) require the presence of a polarizable moiety situated in an anharmonic potential. Our approach to incorporating such properties into self-assembled multilayers involves use of asymmetric α,ω bisphosphonates which meet this requirement by virtue of their chemical structure and binding properties. We have developed and optimized protection and deprotection schemes to allow for oriented layering of these molecules. Characterization by optical ellipsometry and grazing angle X-ray diffraction provides insight on average layer thicknesses and bulk film densities. Second harmonic generation (SHG) intensity from the bulk film is measured to verify NLO activity.