The impact of Pb on the environment and human health and recent restrictions on its use in electronic devices are generating demand for Pb-free piezoelectric materials. Examples are now available commercially, but the full elastic-piezoelectric-dielectric (EPD) matrices needed for device design, including over a range of operating conditions, have not yet been published. The standard IEEE EPD matrix measurement method needs four sample geometries, making it inconvenient and increasing errors. Here, we present an alternative method combining resonant ultrasound spectroscopy with optimization algorithms to measure the EPD matrix from a single exact cube sample. The Levenberg–Marquardt (LM) and Nelder–Mead (NM) optimizations are compared in re...