Silicon nitride films grown by plasma-enhanced chemical vapor deposition (PECVD) are useful for a variety of applications, including anti-reflecting coatings in solar cells, passivation layers, dielectric layers in metal/insulator structures, and diffusion masks. PECVD systems are controlled by many operating variables, including RF power, pressure, gas flow rate, reactant composition, and substrate temperature. The wide variety of processing conditions, as well as the complex nature of particle dynamics within a plasma, makes tailoring SiN film properties very challenging, since it is difficult to determine the exact relationship between desired film properties and controllable deposition conditions. In this study, SiN PECVD modeling using optimized neural networks has been investigated. The deposition of SiN was characterized via a central composite experimental design, and data from this experiment was used to train and optimize feed-forward neural networks using the back-propagation algorithm. From these neural process models, the effect of deposition conditions on film properties has been studied. A recipe synthesis (optimization) procedure was then performed using the optimized neural network models to generate the necessary deposition conditions to obtain several novel film qualities including high charge density and long lifetime. This optimization procedure utilized genetic algorithms, hybrid combinations of genetic algorithm and Powells algorithm, and hybrid combinations of genetic algorithm and simplex algorithm. Recipes predicted by these techniques were verified by experiment, and the performance of each optimization method are compared. It was found that the hybrid combinations of genetic algorithm and simplex algorithm generated recipes produced films of superior quality.