The application of 2D-assisted epitaxy in the growth of freestanding membranes, hybrid 2D/3D heterostructures, and direct integration of highly mismatched materials has sparked significant interest in fields such as electronics, optoelectronics, and quantum devices. This method has been utilized for the growth of variety of materials, including III-N and III-V semiconductor compounds, various oxide compounds, perovskites, metals, and 2D materials, demonstrating its tremendous potential. However, one of its major challenges remains the growth of non-polar materials like Ge. This is mainly due to the minimal interaction between non-polar materials and 2D interface or underlying bulk substrate. This makes the nucleation and crystal orientation of epilayers very difficult, resulting in polycrystalline structures.In this study, we unravel the key mechanisms governing the nucleation and growth of 3D non-polar materials on suspended single-layer graphene (SLG) from real-time observations of the growth by using in-situ Transmission electron microscopy (TEM)[1]. This powerful technique provides a unique opportunity to observe new and yet unexplored phenomena, which are not accessible to the standard ex-situ characterizations. Through direct observations, remote interactions are elucidated between Ge crystals through the graphene layer in double heterostructures of Ge/graphene/Ge. Based on these findings, we implemented a novel approach for growth of non-polar materials by 2D-assisted epitaxy, called “anchor point nucleation”[2]. This method involves the engineering of the SLG substrate, by introducing defects that act as preferential nucleation sited for the epitaxial growth and aid orienting the epilayer by the underlying substrate. Figure 1 illustrates this approach.The engineering of the SLG was achieved through plasma treatment, and the effects of the treatment duration were analyzed by using X-ray photoelectron spectroscopy (XPS) and Raman spectroscopy. Experimental data confirmed the introduction of defects after the treatment, leading to an increase in nucleation sites shown by the increasing number of Ge nuclei on the treated SLG. These observations corroborate the pivotal role of induced defects in the nucleation process, enhancing surface energy and the reactivity of graphene. The high quality of the resulting epitaxial layers is demonstrated through TEM and electron backscatter diffraction (EBSD) characterizations. These findings mark the first demonstration of anchor point nucleation enabling high-quality growth of non-polar semiconductors through 2D-assisted epitaxy.[1] T.M. Diallo et al., Small (2022), 18, 2101890. (https://doi.org/10.1002/smll.202101890)[2] T.M. Diallo, T. Hanuš et al., Small (2023), 20, 2306038 (https://doi.org/10.1002/smll.202306038) Figure 1
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