Discerning element and site-specific fluctuations of the charge-orbital order in Fe 3 O 4 below the Verwey transition
Abstract
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.
- Authors:
-
[2];
[3];
- Univ. of California, San Diego, La Jolla, CA (United States)
- Univ. of California, Davis, CA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); US Air Force Office of Scientific Research (AFOSR); National Science Foundation (NSF)
- OSTI Identifier:
- 1924210
- Report Number(s):
- BNL-224009-2023-JAAM
Journal ID: ISSN 2475-9953; TRN: US2312488
- Grant/Contract Number:
- SC0012704; SC0001805; FA9550-16-1-0026; DMR-1411335; DMR-1902652
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Review Materials
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 1; Journal ID: ISSN 2475-9953
- Publisher:
- American Physical Society (APS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Jahn-Teller effect; orbital order; phase transitions by order
Citation Formats
Hua, Nelson, Li, Jianheng, Hrkac, Stjepan B., Barbour, Andi, Hu, Wen, Mazzoli, Claudio, Wilkins, Stuart, Kukreja, Roopali, Fullerton, Eric E., and Shpyrko, Oleg G. Discerning element and site-specific fluctuations of the charge-orbital order in Fe3O4 below the Verwey transition. United States: N. p., 2023.
Web. doi:10.1103/physrevmaterials.7.014413.
Hua, Nelson, Li, Jianheng, Hrkac, Stjepan B., Barbour, Andi, Hu, Wen, Mazzoli, Claudio, Wilkins, Stuart, Kukreja, Roopali, Fullerton, Eric E., & Shpyrko, Oleg G. Discerning element and site-specific fluctuations of the charge-orbital order in Fe3O4 below the Verwey transition. United States. https://doi.org/10.1103/physrevmaterials.7.014413
Hua, Nelson, Li, Jianheng, Hrkac, Stjepan B., Barbour, Andi, Hu, Wen, Mazzoli, Claudio, Wilkins, Stuart, Kukreja, Roopali, Fullerton, Eric E., and Shpyrko, Oleg G. Tue .
"Discerning element and site-specific fluctuations of the charge-orbital order in Fe3O4 below the Verwey transition". United States. https://doi.org/10.1103/physrevmaterials.7.014413. https://www.osti.gov/servlets/purl/1924210.
@article{osti_1924210,
title = {Discerning element and site-specific fluctuations of the charge-orbital order in Fe3O4 below the Verwey transition},
author = {Hua, Nelson and Li, Jianheng and Hrkac, Stjepan B. and Barbour, Andi and Hu, Wen and Mazzoli, Claudio and Wilkins, Stuart and Kukreja, Roopali and Fullerton, Eric E. and Shpyrko, Oleg G.},
abstractNote = {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.},
doi = {10.1103/physrevmaterials.7.014413},
journal = {Physical Review Materials},
number = 1,
volume = 7,
place = {United States},
year = {Tue Jan 31 00:00:00 EST 2023},
month = {Tue Jan 31 00:00:00 EST 2023}
}
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