Lawrence Berkeley National Laboratory

AB2O4 normal spinels with a magnetic B site can host a variety of magnetic and orbital frustrations leading to spin-liquid phases and field-induced phase transitions. Here, we report the epitaxial growth of (111)-oriented MgCr2O4 thin films. By characterizing the structural and electronic properties of films grown along the (001) and (111) directions, the influence of growth orientation has been studied. Despite distinctly different growth modes observed during deposition, the comprehensive characterization reveals no measurable disorder in the cation distribution nor multivalency issue for Cr ions in either orientation. Contrary to a naive expectation, the (111) stabilized films exhibit a smoother surface and a higher degree of crystallinity than (001)-oriented films. The preference in growth orientation is explained within the framework of heteroepitaxial stabilization in connection to a significantly lower (111) surface energy. These findings open broad opportunities in the fabrication of two-dimensional kagome-triangular heterostructures with emergent magnetic behavior inaccessible in bulk crystals.