Stacking-Selective Epitaxy of Rare-Earth Diantimonides

Deterministic control of the layering configuration of two-dimensional quantum materials plays a central role in studying their emergent electronic properties. Here we demonstrate in-situ control over competing stacking configurations in thin film crystals of the rare-earth diantimonides by synthesizing in proximity to competing structural orders. A crossover between the epitaxially stabilized monoclinic structure and the orthorhombic structure commonly observed in bulk crystals is navigated through three axes; the relative cation/anion ratio, growth temperature, and choice of lanthanide ion, culminating with a comparative magnetotransport study of single-yet-distinct phase CeSb2 films. These results set the stage for an expanded search for hidden stacking configurations in layered compounds which have evaded detection.