Discerning element and site-specific fluctuations of the charge-orbital order in Fe3O4 below the Verwey transition

• Published in: Physical review materials 2023-01, Vol.7 (1)
• Main Authors: Hua, Nelson, Li, Jianheng, Hrkac, Stjepan B., Barbour, Andi, Hu, Wen, Mazzoli, Claudio, Wilkins, Stuart, Kukreja, Roopali, Fullerton, Eric E., Shpyrko, Oleg G.
• Format: Article
• Language: English
• Subjects: CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Jahn-Teller effect; MATERIALS SCIENCE; orbital order; phase transitions by order
• ISSN: 2475-9953; 2475-9953
• DOI: 10.1103/PhysRevMaterials.7.014413

Despite countless experimental probes into magnetite's electronic structure across the Verwey transition Fe3O4, the exact origin of this archetypical metal-insulator transition remains a puzzle. Advanced x-ray diffraction techniques have mostly resolved the monoclinic structure of the insulating phase, including interatomic bond lengths, but the complexity of the charge-orbitally ordered state is difficult to disentangle. Here we combined resonant elastic x-ray scattering and x-ray photon correlation spectroscopy to probe charge-orbital fluctuations in the insulating state of magnetite. By accessing the Bragg forbidden $(00\frac{1}{2})_{c}$ peak at the oxygen K-edge, we complement our previous study on the iron L3 – edge to reveal the dynamics of the iron 3d and oxygen 2p orbital domains. Our new results reveal a decoupling of the orbital correlation lengths between the oxygen 2p states and site-specific iron 3d states, and we further show charge-orbital domain fluctuations at the iron t2g orbital sites of trimeron chains. These results also demonstrate an experimental method capable of distinguishing electronic dynamics between the oxygen ligands and the transition metal that underpins emergent behaviors in complex oxides.