Enhanced Piezoelectric Response in Hybrid Lead Halide Perovskite Thin Films via Interfacing with Ferroelectric PbZr_0.2Ti_0.8O₃

Abstract

We report a more than 10-fold enhancement of the piezoelectric coefficient d₃₃ of polycrystalline CH₃NH₃PbI₃ (MAPbI₃) films when interfacing them with ferroelectric PbZr_0.2Ti_0.8O₃ (PZT). Piezoresponse force microscopy (PFM) studies reveal [Formula: see text] values of 0.3-0.4 pm/V for MAPbI₃ deposited on Au, indium tin oxide, and SrTiO₃ surfaces, with small phase angle fluctuating at length scales smaller than the grain size. In sharp contrast, on samples prepared on epitaxial PZT films, we observe large-scale polar domains exhibiting clear, close to 180° PFM phase contrasts, pointing to polar axes along the film normal. By separating the piezoresponse contributions from the MAPbI₃ and PZT layers, we extract a significantly higher [Formula: see text] of ∼4 pm/V, which is attributed to the enhanced alignment of the MA molecular dipoles promoted by the unbalanced surface potential of PZT. We also discuss the effect of the interfacial screening layer on the preferred polar direction.