Methods of forming a crystalline strontium titanate layer may include providing a substrate with a crystal enhancement surface (e.g., Pt), depositing strontium titanate by atomic layer deposition, and conducting a post-deposition anneal to crystallize the strontium titanate. Large single crystal domains may be formed, laterally extending greater distances than the thickness of the strontium titanate and demonstrating greater ordering than the underlying crystal enhancement surface provided to initiate ALD. Functional oxides, particularly perovskite complex oxides, can be heteroepitaxially deposited over the crystallized STO.