Defining ferroelectric characteristics with reversible piezoresponse: PUND switching spectroscopy PFM characterization

Abstract Detecting ferroelectricity at micro- and nanoscales is crucial for advanced nanomaterials and materials with complicated topography. Switching Spectroscopy Piezoresponse Force Microscopy (SSPFM), which involves measuring piezoelectric hysteresis loops via a scanning probe microscopy tip, is a widely accepted approach to characterize polarization reversal at the local scale and confirm ferroelectricity. However, the local hysteresis loops acquired through this method often exhibit unpredictable shapes, a phenomenon often attributed to the influence of parasitic factors such as electrostatic forces and current flow. Our research has uncovered that the deviation in hysteresis loop shapes can be caused by the spontaneous backswitching occurring after polarization reversal. Moreover, we've determined that the extent of this effect can be exacerbated when employing inappropriate SSPFM waveform parameters, including duration, frequency, and AC voltage amplitude. Notably, the conventional "pulse-mode" SSPFM method has been found to intensify spontaneous backswitching. In response to these challenges, we have redesigned the approach by introducing the positive up – negative down (PUND) method within the “step-mode” SSPFM. This modification allows for effective probing of local piezoelectric hysteresis loops in ferroelectrics with reversible piezoresponse while removing undesirable electrostatic contribution. This advancement extends the applicability of the technique to a diverse range of ferroelectrics, including semiconductor ferroelectrics and relaxors, promising a more reliable and accurate characterization of their properties.