Evolution of Ferroelectric Properties in Sm_<i>x</i>Bi_1–<i>x</i>FeO₃ via Automated Piezoresponse Force Microscopy across combinatorial spread libraries

Combinatorial spread libraries offer an approach to explore the evolution of material properties over broad concentration, temperature, and growth parameter spaces. However, the traditional limitation of this approach is the requirement for the read-out of functional properties across the library. Here we develop automated piezoresponse force microscopy (PFM) for the exploration of combinatorial spread libraries and demonstrate its application in the Sm_<i>x</i>Bi_1-<i>x</i>FeO₃ system with the ferroelectric-antiferroelectric morphotropic phase boundary. This approach relies on the synergy of the quantitative nature of PFM and the implementation of automated experiments that allow PFM-based sampling of macroscopic samples. The concentration dependence of pertinent ferroelectric parameters was determined and used to develop the mathematical framework based on the Ginzburg-Landau theory describing the evolution of these properties across the concentration space. We pose that a combination of automated scanning probe microscope and combinatorial spread library approach will emerge as an efficient research paradigm to close the characterization gap in high-throughput materials discovery. We make the data sets open to the community, and we hope that this will stimulate other efforts to interpret and understand the physics of these systems.