Patterning of large area nanoscale domains in as-grown epitaxial ferroelectric PbTiO3 films

Effective tuning of nanoscale domain structures provides fundamental basis for controlling and engineering of various functionalities in ferroelectric materials. In this work, we demonstrate the precise patterning of nanoscopic domain structures in as-grown epitaxial PbTiO3 (PTO) films by merely introducing an ultrathin pre-patterned doping layer (e.g., Fe-doped PTO). The doping layer can effectively reverse the interfacial built-in bias, consequent to a reversed initial polarization reorientation in the as-grown film, which makes it possible to transfer the nano-patterns in the doping layer into the domain structure of ferroelectric films. For instance, we have successfully fabricated large area ordered array of nanoscale cylindrical domains (downward polarization) embedded in the matrix domain with opposite polarization (upward polarization) in PTO film. These nanoscale cylinder domains also allow deterministic and reversible erasure and creation induced by biased tip scanning. The results provide an effective pathway for on-demand patterning of large area nanoscale domains in the as-grown films, which may find applications in a wide range of nanoelectronic devices.