Magnetic Ordering in Sr₃YCo₄O_10+x

Transition-metal oxides often exhibit complex magnetic behavior due to the strong interplay between atomic-structure, electronic and magnetic degrees of freedom. Cobaltates, especially, exhibit complex behavior because of cobalt's ability to adopt various valence and spin state configurations. The case of the oxygen-deficient perovskite Sr₃YCo₄O_10+x (SYCO) has attracted considerable attention because of persisting uncertainties about its structure and the origin of the observed room temperature ferromagnetism. Here we report a combined investigation of SYCO using aberration-corrected scanning transmission electron microscopy and density functional theory calculations. Guided by theoretical results on Co-O distances projected on different planes, the atomic-scale images of several different orientations, especially of the fully oxygenated planes, allow the unambiguous extraction of the underlying structure. The calculated magnetic properties of the new structure are in excellent agreement with the experimental data.