Publication date: 21st July 2025
The switchable bistable polarization in ferroelectrics allows for the binary control of optical, electronic, and catalytic properties that are essential for a wide range of applications. Going beyond the limitation of a binary remanent polarization and using that for evoking strongly non-linear material responses holds great promise for emerging spintronic and neuromorphic concepts. Here, we demonstrate that we can arbitrarily set the magnitude of the remanent ferroelectric polarization at the nanoscale in epitaxial PbZr0.52Ti0.48O3 thin films with a single DC bias. By driving the ferroelectric system towards an instability near the PZT morphotropic phase boundary and controlling the resulting softness via epitaxial strain, we favor the formation of decoupled nanometric 180° domains that exhibit a broad coercive field distribution. Using in-situ optical second harmonic generation and X-ray diffraction, we investigate the emergence of the nanoscopic domain configuration. We then use piezoresponse force microscopy to demonstrate the possibility to locally and reversibly modulate the remanent polarization continuously between depolarized and saturated, while preserving the nanoscopic length scale of the domains. We highlight the direct technological relevance of nanoscale non-binary polarization switching, by showing first, the voltage-controlled tunability of the nonlinear optical response in our films and second, the quasi-continuous tunability of the tunnel electroresistance in ferroelectric tunnel junctions.
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