Long-Range Orbital Hybridization in Remote Epitaxy: The Nucleation Mechanism of GaN on Different Substrates via...

Remote epitaxy is a very promising technique for the preparation of single-crystal thin films of flexibly transferred III-V group semiconductors. However, the epilayer nucleation mechanism of remote epitaxy and the epilayer-substrate interface interactions on both sides of graphene are not well-understood. In this study, remote homo- and heteroepitaxy of GaN nucleation layers (NLs) were performed by metal organic chemical vapor deposition on GaN, sapphire (Al₂O₃), and AlN substrates with transferred single-layer graphene, respectively. The results show that the interface damage of SLG/GaN at high temperature is difficult for us to achieve the remote homoepitaxy of GaN. Therefore, we explored the nucleation mechanism of remote heteroepitaxy of GaN on SLG/Al₂O₃ and SLG/AlN substrates. Nucleation density, surface coverage, diffusion coefficient, and scaled nucleation density were used to quantify the differences in nucleation information of GaN grown on different polar substrates. Using high-resolution X-ray diffraction and high-resolution transmission electron microscopy analysis, we revealed the interfacial orientation relationship and atomic arrangement distribution between the GaN NLs and substrates on both sides of the SLG. The electrostatic potential effect and adsorption ability of the substrates were further investigated by first-principles calculations based on density functional theory, revealing the principle that the substrate polarity affects the atomic nucleation density. The partial density of states shows that there is long-range orbital hybridization of the electronic states of the substrate and adsorbed atoms in remote epitaxy, and the crystal properties of the substrate play an important role in the in-plane orientation relationship of the NL and substrate across the SLG. The abovementioned results reveal the nature of remote epitaxy and broaden the perspective for the rapid and large-area preparation of single-crystal GaN films.