Polarizing ultrathin ferroelectric BaTiO3 films through interfacial layer polarization

Abstract

An important requirement for the integration of ferroelectric thin films into devices is deterministic control of the polarization state in films of only a few unit cells in thickness. Here, we utilize the charged atomic planes of (001)-oriented SmNiO$_3$ (SNO) buffer layers as a polarizing template to stabilize the polarization in ferroelectric BaTiO$_3$ (BTO) model system thin films. We show that an upwards (downwards) oriented polarization is achieved by selection of the [SmO]$^+$ ([NiO$_2$]$^-$) buffer termination. Most importantly, the charged atomic planes of SNO suppress the depolarizing-field-induced critical thickness in BTO, and we record the emergence of a net polarization in our BTO films from the first unit cell deposited. Our experiments, guided by density-functional-theory (DFT) calculations, further highlight the impact of charged defects on the polarizing effectiveness of the SNO buffer. Specifically, oxygen vacancies counteract the polarizing field of the negatively charged, [NiO$_2$]$^-$-terminated surface of the SNO buffer. Our findings provide important insights into the interplay of defect chemistry and polarizing interfaces to stabilize ferroelectric polarization down to the single-unit-cell limit.