Novel Approach to High κ (∼59) and Low EOT (∼3.8 Å) near the Morphotrophic Phase Boundary with AFE/FE (ZrO 2 /HZO) Bilayer Heterostructures and High-Pressure Annealing.

We present herewith a novel approach of equally thick AFE/FE (ZrO ₂ /HZO) bilayer stack heterostructure films for achieving an equivalent oxide thickness (EOT) of 4.1 Å with a dielectric constant (κ) of 56 in complementary metal-oxide semiconductor (CMOS) compatible metal-ferroelectric-metal (MFM) capacitors using a high-pressure annealing (HPA) technique. The low EOT and high κ values were achieved by careful optimization of AFE/FE film thicknesses and HPA conditions near the morphotropic phase boundary (MPB) after field cycling effects. Stable leakage current density ( J < 10 ^-7 A/cm ² at ±0.8 V) was found at 3/3 nm bilayer stack films (κ = 56 and EOT = 4.1 Å) measured at room temperature. In comparison with previous work, our remarkable achievement stems from the interfacial coupling between FE and AFE films as well as a high-quality crystalline structure formed by HPA. Kinetically stabilized hafnia films result in a small grain size in bilayer films, leading to reducing the leakage current density. Further, a higher κ value of 59 and lower EOT of 3.4 Å were found at 333 K. However, stable leakage current density was found at 273 K with a high κ value of 53 and EOT of 3.85 Å with J < 10 ^-7 A/cm ² . This is the lowest recorded EOT employing hafnia and TiN electrodes that are compatible with CMOS, and it has important implications for future dynamic random access memory (DRAM) technology.