Ferroelastic Nanodomain-mediated Mechanical Switching of Ferroelectricity in Thick Epitaxial Films

Mechanical switching of ferroelectric polarization, typically realized via a scanning probe, holds promise in (multi)ferroic device applications. Whereas strain gradient-associated flexoelectricity has been regarded to be accountable for mechanical switching in ultrathin (<10 nm) films, such mechanism can hardly be extended to thicker materials due to intrinsic short operating lengths of flexoelectricity. Here, we demonstrate robust mechanical switching in a100 nm thick Pb(Zr0.2Ti0.8)O3 epitaxial films with a characteristic microstructure consisting of nanosized ferroelastic domains. Through a combination of multiscale structural characterizations, piezoresponse force microscopy, and phase-field simulations, we reveal that the ferroelastic nanodomains effectively mediate the 180° switching nucleation in a dynamical manner during tip scanning. Coupled with microstructure engineering, this newly revealed mechanism could boost the utility of mechanical switching through extended material systems. Our results also provide insight into competing polarization switching pathways in complex ferroelectric materials, essential for understanding their electromechanical response.