Thin films of organic nonlinear optical materials are deposited by vapor deposition from sublimation sources in vacuum. Chemical bonding and polymerization of these materials is studied during deposition to try to improve the physical properties of these materials relative to those of the molecular crystals. Excitation of the growing film by chemical adsorption and ion or photon excitation is used. The nonlinear organic materials that are studied are urea, POM and MAP. Amino acids are additionally studied.