Direct Observation of Oxide Ion Dynamics in La2Mo2O9 on the Nanosecond Timescale

Peet, J. R.; Fuller, C. A.; Frick, B.; Zbiri, M.; Piovano, A.; Johnson, M. R.; Radosavljevic Evans, I.

Abstract

Quasielastic neutron scattering (QENS), underpinned by ab-initio molecular dynamics (AIMD) simulations, has been used to directly observe oxide ion dynamics in solid electrolyte La2Mo2O9 on the nanosecond timescale, the longest timescale probed in oxide ion conductors by neutron scattering to date. QENS gives the activation energy of 0.61(5) eV for this process, while AIMD simulations reveal that the exchange processes, which ultimately lead to long-range oxide ion diffusion in La2Mo2O9, rely on the flexibility of the coordination environment around Mo6+, with oxide ions jumps occurring between vacant sites both within and between Mo coordination spheres. Simulations also differentiate between the crystallographic sites which participate in the oxide ion exchange processes, offering the first atomic-level understanding of the oxide ion dynamics in La2Mo2O9, which is consistent with the macroscopic experimental observations on this material.

Citation

Peet, J. R., Fuller, C. A., Frick, B., Zbiri, M., Piovano, A., Johnson, M. R., & Radosavljevic Evans, I. (2017). Direct Observation of Oxide Ion Dynamics in La2Mo2O9 on the Nanosecond Timescale. Chemistry of Materials, 29(7), 3020-3028. https://doi.org/10.1021/acs.chemmater.6b05507

• Journal Article Type: Article
• Acceptance Date: Mar 16, 2017
• Online Publication Date: Mar 24, 2017
• Publication Date: Apr 11, 2017
• Deposit Date: Mar 23, 2017
• Publicly Available Date: Mar 16, 2018
• Journal: Chemistry of Materials
• Print ISSN: 0897-4756
• Electronic ISSN: 1520-5002
• Publisher: American Chemical Society
• Peer Reviewed: Peer Reviewed
• Volume: 29
• Issue: 7
• Pages: 3020-3028
• DOI: https://doi.org/10.1021/acs.chemmater.6b05507
• Public URL: https://durham-repository.worktribe.com/output/1361507