Pyroelectric materials have been widely used for a range of thermal-related applications including thermal imaging/sensing, waste heat energy conversion, and electron emission. In general, the figures of merit for applications of pyroelectric materials are proportional to the pyroelectric coefficient and inversely proportional to the dielectric permittivity. In this context, we explore single-layer and compositionally graded PbZr1-xTixO3 thin-film heterostructures as a way to independently engineer the pyroelectric coefficient and dielectric permittivity of materials and increase overall performance. Compositional gradients in thin films are found to produce large strain gradients which generate large built-in potentials in the films that can reduce the permittivity while maintaining large pyroelectric response. Routes to enhance the figures of merit of pyroelectric materials by 3-12 times are reported, and comparisons to standard materials are made
