High-Performance TiO₂/ZrO₂/TiO₂ Thin Film Capacitor by Plasma-Assisted Atomic Layer Annealing

Although laminate structures are widely used in electrostatic capacitors, unavoidable heterogeneous interfaces often deteriorate the dielectric properties by impeding film crystallization. In this study, a TiO₂/ZrO₂/TiO₂ (TZT) laminate structure, where upper-TiO₂ deposited on the heterogeneous interface was crystallized by plasma-assisted atomic layer annealing (ALA), was investigated. ALA effectively induced the phase transition of the upper-TiO₂ from the amorphous or anatase phase to the rutile phase, leading to an increase in the dielectric constant, whereas the ZrO₂ blocking interlayer maintained the amorphous phase owing to the extremely localized effect of ALA. Consequently, through the layer-by-layer phase control of ALA, the dielectric constant of the upper-TiO₂ was enhanced by 25% by applying ALA, leading to an increase in a capacitance density of 27% of the TZT capacitor, whereas a low leakage current density of ∼10^-8 A/cm² was maintained (at 1 V). In addition, the TZT capacitor on three-dimensional structures (aspect ratio of 5:1) shows a high capacitance density of up to 461 nF/mm² owing to ALA.