Abstract: A layer-by-layer deposition process for a thin film having a polyelectrolyte and a complementary species includes calibrating a buffered polyelectrolyte solution and a buffered rinse solution, depositing a polyelectrolyte layer on a substrate, and depositing a complementary species layer on the polyelectrolyte layer. Depositing a polyelectrolyte layer includes applying the buffered polyelectrolyte solution to the substrate and applying the buffered rinse solution to the substrate after the buffered polyelectrolyte solution has been applied. Depositing a complementary species layer includes applying a complementary species mixture to the substrate and applying a complementary species rinse solution to the substrate after the complementary species mixture has been applied.