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Polarization dynamics in ferroelectric materials are explored via theautomated experiment in Piezoresponse Force Spectroscopy. A BayesianOptimization framework for imaging is developed and its performance for avariety of acquisition and pathfinding functions is explored using previouslyacquired data. The optimized algorithm is then deployed on an operationalscanning probe microscope (SPM) for finding areas of large electromechanicalresponse in a thin film of PbTiO3, with metrics showing gains of ~3x in thesampling efficiency. This approach opens the pathway to perform more complexspectroscopies in SPM that were previously not possible due to time constraintsand sample stability, tip wear, and/or stochastic sample damage that occurs atspecific, a priori unknown spatial positions. Potential improvements to theframework to enable the incorporation of more prior information and improveefficiency further are discussed.

Autonomous Experiments in Scanning Probe Microscopy and Spectroscopy: Choosing Where to Explore Polarization Dynamics in Ferroelectrics