Beyond traditional heteroepitaxy, 2D‐materials‐assisted epitaxy opens opportunities to revolutionize future material integration methods. However, basic principles in 2D‐material‐assisted nitrides’ epitaxy remain unclear, which impedes understanding the essence, thus hindering its progress. Here, the crystallographic information of nitrides/2D material interface is theoretically established, which is further confirmed experimentally. It is found that the atomic interaction at the nitrides/2D material interface is related to the nature of underlying substrates. For single‐crystalline substrates, the heterointerface behaves like a covalent one and the epilayer inherits the substrate's lattice. Meanwhile, for amorphous substrates, the heterointerface tends to be a van der Waals one and strongly relies on the properties of 2D materials. Therefore, modulated by graphene, the nitrides’ epilayer is polycrystalline. In contrast, single‐crystalline GaN films are successfully achieved on WS2. These results provide a suitable growth‐front construction strategy for high‐quality 2D‐material‐assisted nitrides’ epitaxy. It also opens a pathway toward various semiconductors heterointegration.
The key mechanism lies in that the potential field of substrates can penetrate Gr to govern the lattice arrangement of epilayers, while Gr weakens the substrateepilayer coupling. [2e,3] Up until now, most of the epitaxy of nitrides via Gr is performed on heterogeneous substrates, such as sapphire. [2a,d,4] As shown in Table S1, Supporting Information, large lattice and thermal mismatches between sapphire and nitrides still exist, which inevitably leads to a high density of dislocations in nitrides, and thus, degrades the performance of optoelectronic devices by forming non-radiation centers and leakage channels. [2d,5] Thus, the practical application of Gr-assisted epitaxy of nitrides for high-performance nitride-based optoelectronic devices is still hindered.
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