Spin-charge coupling and decoupling in perovskite-type iron oxides (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$

TL;DR

This study reveals spin-charge decoupling and a competing antiferromagnetic phase in perovskite iron oxides with Ba substitution, expanding understanding of magnetic and charge order interactions in these materials.

Contribution

It reports the discovery of spin-charge decoupling and a new antiferromagnetic phase in (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$, highlighting effects of Ba substitution on phase behavior.

Findings

Ba substitution reduces SCO critical temperature.

Spin-charge decoupling occurs for x > 0.75.

G-type AFM phase appears as a high-temperature metastable state.

Abstract

The perovskite-type iron oxide Sr$_{2/3}$La$_{1/3}$FeO$_3$ is known to show characteristic spin-charge ordering (SCO), where sixfold collinear spin ordering and threefold charge ordering are coupled with each other. Here, we report the discovery of a spin-charge decoupling and an antiferromagnetic (AFM) state competing with the SCO phase in perovskites (Sr$_{1-x}$Ba$_x$)$_{2/3}$La$_{1/3}$FeO$_3$. By comprehensive measurements including neutron diffraction, M$\"{o}$ssbauer spectroscopy, and x-ray absorption spectroscopy, we found that the isovalent Ba$^{2+}$ substitution systematically reduces the critical temperature of the SCO phase and additionally yields the spin-charge decoupling in $x$ > 0.75. Whereas the ground state remains in the SCO phase in the whole $x$ region, an unexpected G-type AFM phase with incoherent charge ordering or charge fluctuation appears as the high-temperature phase in the range of $x$ > 0.75. Reflecting the competing nature between them, the G-type AFM phase partially exists as a metastable state in the SCO phase at low temperatures. We discuss the origin of the spin-charge decoupling and the emergence of the G-type AFM phase with charge fluctuation in terms of the bandwidth reduction by the Ba substitution.