Remote epitaxy is a recently discovered type of epitaxy, wherein single-crystalline thin films can be grown on graphene-coated substrates following the crystallinity of the substrate via remote interaction through graphene. Although remote epitaxy provides a pathway to form freestanding membranes by controlled exfoliation of grown film at the graphene interface, implementing remote epitaxy is not straightforward because atomically precise control of interface is required. Here, we unveil the role of the graphene–substrate interface on the remote epitaxy of GaAs by investigating the interface at the atomic scale. By comparing remote epitaxy on wet-transferred and dry-transferred graphene, we show that interfacial oxide layer formed at the graphene–substrate interface hinders remote interaction through graphene when wet-transferred graphene is employed, which is confirmed by an increase of interatomic distance through graphene and also by the formation of polycrystalline films on graphene. On the other hand, when dry-transferred graphene is employed, the interface is free of native oxide, and single-crystalline remote epitaxial films are formed on graphene, with the interatomic distance between the epilayer and the substrate matching with the theoretically predicted value. The first atomic layer of the grown film on graphene is vertically aligned with the top layer of the substrate with these atoms having different polarities, substantiating the remote interaction of adatoms with the substrate through graphene. These results directly show the impact of interface properties formed by different graphene transfer methods on remote epitaxy.

Remote epitaxy, which was discovered and reported in 2017, has seen a surge of interest in recent years. Although the technology seemed to be difficult to reproduce by other labs at first, remote epitaxy has come a long way and many groups are able to consistently reproduce the results with a wide range of material systems including III-V, III-N, wide band-gap semiconductors, complex-oxides, and even elementary semiconductors such as Ge. As with any nascent technology, there are critical parameters which must be carefully studied and understood to allow wide-spread adoption of the new technology. For remote epitaxy, the critical parameters are the (1) quality of two-dimensional (2D) materials, (2) transfer or growth of 2D materials on the substrate, (3) epitaxial growth method and condition. In this review, we will give an in-depth overview of the different types of 2D materials used for remote epitaxy reported thus far, and the importance of the growth and transfer method used for the 2D materials. Then, we will introduce the various growth methods for remote epitaxy and highlight the important points in growth condition for each growth method that enables successful epitaxial growth on 2D-coated single-crystalline substrates. We hope this review will give a focused overview of the 2D-material and substrate interaction at the sample preparation stage for remote epitaxy and during growth, which have not been covered in any other review to date. Graphical Abstract

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