Ultralow Tip‐Force Driven Sizable‐Area Domain Manipulation through Transverse Flexoelectricity

Abstract Deterministic control of ferroelectric domain is critical in the ferroelectric functional electronics. Ferroelectric polarization can be manipulated mechanically with a nano‐tip through flexoelectricity. However, it usually occurs in a very localized area in ultrathin films, with possible permanent surface damage caused by a large tip‐force. Here it is demonstrated that the deliberate engineering of transverse flexoelectricity offers a powerful tool for improving the mechanical domain switching. Sizable‐area domain switching under an ultralow tip‐force can be realized in suspended van der Waals ferroelectrics with the surface intact, due to the enhanced transverse flexoelectric field. The film thickness range for domain switching in suspended ferroelectrics is significantly improved by an order of magnitude to hundreds of nanometers, being far beyond the limited range of the substrate‐supported ones. The experimental results and phase‐field simulations further reveal the crucial role of the transverse flexoelectricity in the domain manipulation. This large‐scale mechanical manipulation of ferroelectric domain provides opportunities for the flexoelectricity‐based domain controls in emerging low‐dimensional ferroelectrics and related devices.