Strongly Coupled Magnetic and Electronic Transitions in Multivalent Strontium Cobaltites

The topotactic phase transition in SrCoO(x) (x = 2.5–3.0) makes it possible to reversibly transit between the two distinct phases, i.e. the brownmillerite SrCoO(2.5) that is a room-temperature antiferromagnetic insulator (AFM-I) and the perovskite SrCoO(3) that is a ferromagnetic metal (FM-M), owing to their multiple valence states. For the intermediate x values, the two distinct phases are expected to strongly compete with each other. With oxidation of SrCoO(2.5), however, it has been conjectured that the magnetic transition is decoupled to the electronic phase transition, i.e., the AFM-to-FM transition occurs before the insulator-to-metal transition (IMT), which is still controversial. Here, we bridge the gap between the two-phase transitions by density-functional theory calculations combined with optical spectroscopy. We confirm that the IMT actually occurs concomitantly with the FM transition near the oxygen content x = 2.75. Strong charge-spin coupling drives the concurrent IMT and AFM-to-FM transition, which fosters the near room-T magnetic transition characteristic. Ultimately, our study demonstrates that SrCoO(x) is an intriguingly rare candidate for inducing coupled magnetic and electronic transition via fast and reversible redox reactions.