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Epitaxial lift-off techniques, which aim to separate ultrathin single-crystalline epitaxial layers off of the substrate, are becoming increasingly important due to the need of lightweight and flexible devices for heterogeneously integrated ultracompact semiconductor platforms and bioelectronics. Remote epitaxy is a relatively newly discovered epitaxial lift-off technique that allows substrate-seeded epitaxial growth of ultrathin films through few layers of graphene. This universal epitaxial lift-off technique allows freestanding single-crystal membrane fabrication very quickly at low cost. However, the conventional method of remote epitaxy requires transfer of graphene grown on another substrate to the target single-crystalline substrate, which results in organic and metallic residues as well as macroscopic defects such as cracks and wrinkles, significantly reducing the yield of remote epitaxy. Here, we show that direct growth of thick graphene on the target single-crystalline substrate (SrTiO3 for this study) followed by atomic layer etching (ALE) of the graphene layers create a defect- and residue-free graphene surface for high yield remote epitaxy. We find that the ALE efficiently removes one atomic layer of graphene per cycle, while also clearing multi-dots (clumps of carbon atoms) that form during nucleation of the graphene layers. Our results show that direct-grown graphene on the desired substrate accompanied by ALE might potentially be an ideal pathway toward commercialization of 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

Complex-oxide materials are gaining a tremendous amount of interest in the semiconductor materials and device community as they hold many useful intrinsic physical properties such as ferro/piezoelectricity, pyroelectricity, ferromagnetism, as well as magnetostriction and other properties suitable for energy storage elements. Complex-oxides can also be complemented with conventional semiconductor-based devices or used by themselves to realize state-of-the-art electronic/photonic/quantum information devices. However, because complex-oxide materials have vastly different crystalline structures and lattice constant difference compared to conventional semiconductor devices (such as Si or III-V/III-N materials), integration of complex-oxides onto conventional semiconductor platforms has been difficult. Thus, there has been constant efforts to produce freestanding single-crystalline complex-oxide thin films such that these films can be transferred and integrated together with device platforms based on other materials. This review will provide a comprehensive review on single-crystalline complex-oxide membranes technology developed thus far: how they are synthesized, methods to release them from the substrate, and their outstanding properties and applications.