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

Institutions

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
Controls
|||
ALL TIME
JAN
FEB
MAR
APR
MAY
JUN
JUL
AUG
SEP
OCT
article

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

Hideo Hosono, Soshi Iimura, Keiga Fukui, Soshi Takeshita et al.
Physical review. B./Physical review. B
Solid-state spectroscopy and crystallography
article

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

Hideo Hosono, Soshi Iimura, Keiga Fukui, Soshi Takeshita, R. Kadono, A. Koda, Hirotaka Okabe, Anonymous, K. M. Kojima
article en

Abstract

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.

Physical review. B./Physical review. BVol. 113(6)
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)
Openalex Percentile: Top 70%
Solid-state spectroscopy and crystallography
AI Navigator

Ask Laika to Summarize, Analyze, and Connect papers live on the map.

Summarize Papers & Methodologies

Extract key findings, datasets, and comparative methods across publications.

Benchmark Rankings & Visual Analytics

Rank top research institutions, authors, funders, topics, and journals by Field-Weighted Citation Impact (FWCI) and paper volume with instant charts.

Connect Distant Disciplines

Bridge topological clusters on the map to find hidden collaborative intersections.