Tuning Negative Capacitance in PbZr0.2Ti0.8O3/SrTiO3 Heterostructures via Layer Thickness Ratio

Abstract

In this work, we exploit the ferroelectric-dielectric layer thickness ratio r as an effective tuning parameter to control the ferroelectric polarization and transient negative capacitance (NC) state in epitaxial ${\mathrm{Pb}\mathrm{Zr}}_{0.2}{\mathrm{Ti}}_{0.8}{\mathrm{O}}_{3}/{\mathrm{Sr}\mathrm{Ti}\mathrm{O}}_{3}$ bilayer heterostructures. The remnant polarization decreases monotonically with decreasing r, with the system exhibiting an abrupt transition from ferroelectric to dielectric dominated behavior at a critical ratio ${r}_{c}$ of 8 to 7, which is consistent with the evolution of the free-energy profile modeled via Landau theory. For samples with large r, the polarization switching dynamics during the transient NC regime can be well described by the nucleation and growth model, with the narrow distribution of the characteristic switching time (${t}_{0}$) pointing to a domain-wall-motion-limited behavior. Right below ${r}_{c}$, we observe a significantly broadened distribution of ${t}_{0}$, which can be attributed to the emergence of a multidomain state. The transient NC mode is quenched in samples with r 6, confirming that the ferroelectric order is suppressed. Our study provides critical information for optimizing the materials design for complex oxide-based NC transistors, paving the path for their application in low-power nanoelectronics.