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Anionic ordering is a promising route to engineer physical properties infunctional heteroanionic materials. A central challenge in the study ofanion-ordered compounds lies in developing robust synthetic strategies tocontrol anion occupation and in understanding the resultant implications forelectronic structure. Here, we show that epitaxial strain induces preferentialoccupation of F and O on the anion sites in perovskite oxyfluoride SrMnO2.5-dFgfilms grown on different substrates. Under compressive strain, F tends to takethe apical-like sites, which was revealed by F and O K-edge linearly polarizedx-ray absorption spectroscopy and density functional theory calculations,resulting in an enhanced c-axis expansion. Under tensile strain, F tends totake the equatorial-like sites, enabling the longer Mn-F bonds to lie withinthe plane. The anion ordered oxyfluoride films exhibit a significant orbitalpolarization of the 3d electrons, distinct F-site dependence to their valenceband density of states, and an enhanced resistivity when F occupies theapical-like anion site compared to the equatorial-like site. By demonstrating ageneral strategy for inducing anion-site order in oxyfluoride perovskites, thiswork lays the foundation for future materials design and synthesis efforts thatleverage this greater degree of atomic control to realize new polar orquasi-two-dimensional materials.

Strain-induced anion ordering in perovskite oxyfluoride films