Domain Matching Strategy for Orientation Control of van der Waals Epitaxial Perovskite Thin Films

The advantages of van der Waals epitaxy have attracted great interest because they can meet the requirements that conventional epitaxy struggles to satisfy. The weak adatom-substrate interaction without directional covalent bonding drastically relaxes the lattice matching limitation. However, the weak adatom-substrate interaction also leads to ineffectiveness in directing the crystal growth structure, limiting it to one orientation in epitaxial growth. In this work, we propose a domain matching strategy to guide the perovskite-type crystal epitaxial growth on 2D substrates, and we have demonstrated selective deposition of highly (001)-, (110)-, and (111)-oriented epitaxial Fe₄N thin films on mica substrates using applicable transition structure design. Our work makes it possible to achieve and control different orientations of van der Waals epitaxy on the same substrate.