Framework Short-Range Order Observed in a Spinel-Type Li Superionic Conductor
Solid-state superionic conductors are characterized by rich structural disorders. Though structural complexities are central to their functionalities, they often give rise to short-range order that eludes detection by conventional diffraction-based techniques and is thus overlooked in establishing precise structure-property relationships. In this work, we synthesized single crystals of a recently discovered lithium (Li) superionic conductor Li<sub>16.2(1)</sub>In<sub>9.00(2)</sub>Sn<sub>1.10(1)</sub>O<sub>23.8</sub> (LISO) for in-depth characterizations of structural subtleties. LISO exhibits an unusual spinel-like phase with significant Li overstoichiometry and a face-sharing Li network. Single-crystal neutron diffraction confirms significant Li disorder, as manifested in Li site splitting and partial occupancy. More importantly, synchrotron diffuse scattering combined with 3D-ΔPDF analysis and Monte Carlo simulations reveal short-range order in the nonalkali framework that might contribute to the phase stability and ionic conductivity. This work showcases an example in which subtle local energetics can be directly visualized in structurally disordered ionic conductors.
Authors
- Satya Kushwaha (ORCID: https://orcid.org/0000-0002-3169-969X)
- Gopalakrishnan Sai Gautam (ORCID: https://orcid.org/0000-0002-1303-0976)
- Matthew Krogstad (ORCID: https://orcid.org/0000-0002-8505-5945)
- Huiwen Ji (ORCID: https://orcid.org/0000-0001-8091-9428)
- Renu Subramanian
- Birender Singh (ORCID: https://orcid.org/0000-0002-9640-0070)
- Kenneth S. Burch (ORCID: https://orcid.org/0000-0002-7541-0245)
- Caleb Ramette (ORCID: https://orcid.org/0000-0002-0694-9327)
- Erick A. Lawrence (ORCID: https://orcid.org/0000-0003-0819-1895)
- Bin Liu (ORCID: https://orcid.org/0000-0003-1569-2604)
- Jue Liu (ORCID: https://orcid.org/0000-0002-0338-2257)
- Xiaoping Wang
- Paul Cardon
- Chao-Chun Wei
- Yu Chen
- Maxim Avdeev
- Christina M. Hoffmann
Institutions
- Boston College (US)
- Argonne National Laboratory (US)
- Oak Ridge National Laboratory (US)
- Australian Nuclear Science and Technology Organisation (AU)
- Johns Hopkins University (US)
- Lawrence Berkeley National Laboratory (US)
- University of California, Santa Barbara (US)
- University of Utah (US)
- Foundry (United Kingdom) (GB)
- Accelerated Ag Technologies (United States) (US)
- Advanced Photonix (United States) (US)
- Molecular Foundry
- Advanced Photon Source
- Indian Institute of Science Bangalore (IN)
- University of California, Berkeley (US)
Publication Details
- Journal
- Journal of the American Chemical Society
- Published
- 2026-02-23
- DOI
- https://doi.org/10.1021/jacs.5c12231
- Primary Topic
- Advanced Battery Materials and Technologies
- Type
- article
- Field-Weighted Citation Impact
- 0.00