Theoretical Insight into the Band Alignment at High-κ Oxide XO/Diamond (X = Hf and Zr) Interfaces with a SiO Interlayer for MOS Devices.

Diamond has become a promising candidate for high-power devices based on its ultrawide bandgap and excellent thermoelectric properties, where an appropriate gate dielectric has been a bottleneck hindering the development of diamond devices. Herein, we have systematically investigated the structural arrangement and electronic properties of diamond/high-κ oxide (HfO, ZrO) heterojunctions by first-principles calculations with a SiO interlayer. Charge analysis reveals that the C-Si bonding interface attracts a large amount of charge concentrated at the diamond interface, indicating the potential for the formation of a 2D hole gas (2DHG). The diamond/HfO and diamond/ZrO heterostructures exhibit similar "Type II" band alignments with VBOs of 2.47 and 2.21 eV, respectively, which is consistent with experimental predictions. The introduction of a SiO dielectric layer into the diamond/SiO/high-κ stacks exhibits the typical "Type I″ straddling band offsets (BOs). In addition, the wide bandgap SiO interlayer keeps the valence band maximum (VBM) and conduction band minimum (CBM) in the stacks away from those of diamond, effectively confining the electrons and holes in MOS devices. This work exhibits the potential of SiO/high-κ oxide gate dielectrics for diamond devices and provides theoretical insights into the rational design of high-quality gate dielectrics for diamond-based MOS device applications.