Relationship between local hydride ion dynamics and ionic conductivity in <mml:math xmlns:mml="http://www.w3.org/1998/Math/MathML"> <mml:mrow> <mml:msub> <mml:mi>LaH</mml:mi> <mml:mrow> <mml:mn>3</mml:mn> <mml:mo>−</mml:mo> <mml:mn>2</mml:mn> <mml:mi
We performed muon spin rotation and relaxation ($μ$SR) experiments to investigate the microscopic mechanism behind the high ionic conductivity ($σ$) exhibited by hydride (H$^-$) ions in lanthanum hydroxide LaH$_{3-2x}$O$_x$. The $μ$SR spectra observed at 5--300 K in a sample with $x\approx0.25$ consist primarily of two components which are attributed to muons occupying tetrahedral (Tet) and octahedral (Oct) sites common to H$^-$. The spectra also indicate that muons at the Oct sites (Mu$_{\rm O}$) appear nearly stationary in the time scale of $μ$SR ($\sim$10$^{-5}$ s), whereas those at the Tet sites (Mu$_{\rm T}$) are subject to the fluctuating local fields. The cusp-like peak in the fluctuation rate around 160 K and the decrease in linewidth at higher temperatures probed by Mu$_{\rm T}$ suggest that the jump motion of both Mu$_{\rm T}$ (via the vacant Oct sites) and surrounding Oct-site H$^-$ contributes to spin relaxation and that the fluctuation frequency is widely distributed. These results indicate that the implanted Mu behave as Mu$^-$ and that the jump motion of Mu$^-$/H$^-$ is restricted by the availability of nearby vacant sites. On the other hand, the activation energy for the jump is estimated to be 0.11(3) eV, which is significantly different from $\sim$1.3 eV evaluated from the temperature dependence of $σ$ at high temperatures ($\gtrsim400$ K). In our attempt to resolve this discrepancy, we discuss problems inherent in interpreting $σ$ using the Arrhenius equation, and demonstrate that the behavior of H$^-$ ions can be better explained as a viscous fluid exhibiting a glass transition.
Authors
- Hideo Hosono (ORCID: https://orcid.org/0000-0001-9260-6728)
- Soshi Iimura (ORCID: https://orcid.org/0000-0003-3270-155X)
- Keiga Fukui (ORCID: https://orcid.org/0000-0002-5659-7200)
- Soshi Takeshita (ORCID: https://orcid.org/0000-0002-4747-1980)
- R. Kadono (ORCID: https://orcid.org/0000-0002-0915-2727)
- A. Koda (ORCID: https://orcid.org/0000-0002-4453-4472)
- Hirotaka Okabe (ORCID: https://orcid.org/0000-0001-7170-0117)
- Anonymous
- K. M. Kojima
Institutions
- Tokyo Institute of Technology (JP)
- High Energy Accelerator Research Organization (JP)
- The Graduate University for Advanced Studies, SOKENDAI (JP)
- National Institute for Materials Science (JP)
- Shanghai Institute for Science of Science (CN)
- EarthTech International (United States) (US)
- Institute of Science Tokyo (JP)
Publication Details
- Journal
- Physical review. B./Physical review. B
- Published
- 2026-02-03
- DOI
- https://doi.org/10.1103/ll61-rx4f
- Primary Topic
- Solid-state spectroscopy and crystallography
- Type
- article
- Field-Weighted Citation Impact
- 0.00