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.