Order, Disorder, and Dynamics in Brownmillerite Sr₂Fe₂O₅

The room-temperature structure of brownmillerite-type Sr₂Fe₂O₅ remains controversial, despite numerous published crystallographic studies utilizing X-ray, neutron, and electron diffraction data collected on single-crystalline and powder samples. The main disagreements concern the ordering of twisted FeO₄ tetrahedral chains within and between the layers stacked along the <i>b</i> axis, and the impact of this ordering on oxide-ionic conductivity. Here, we present new data along with a reinterpretation of previously published diffraction images, including the reassignment of satellite reflections, which harmonize the results of past studies in a unified description of tetrahedral chain ordering in Sr₂Fe₂O₅ at length scales relevant to X-ray and neutron diffraction. Implications for the prevailing model of oxide ion transport in this material are also discussed.