Computational screening of amorphous lithium trivalent-metal chloride solid-state electrolytes
Abstract
Amorphous solid-state electrolytes (SSEs) are attractive candidates for safe, high-energy-density all-solid-state batteries. The recent discovery that amorphous LiTaCl6 and LiNbCl6 reach room-temperature ionic conductivities above 10 mS cm−1 with activation energies below 0.2 eV has spurred a broad search for new amorphous halide Li conductors. Here we report a computational screening of amorphous lithium trivalent-metal chlorides (Li-M(III)-Cl) using molecular dynamics driven by a universal machine-learning force field. For the sixteen Li-M(III)-Cl compositions spanning fifteen rare-earth elements and indium, all phases exhibit fast room-temperature Li+ diffusion, with diffusivities of roughly $2−5 \times 10^{-7}$ cm2 s−1. After scaling the conductivity versus diffusivity relation to an experimental LiTaCl6 reference, the estimated room-temperature conductivities range from 7.7 mS cm−1 for amorphous Li3InCl6 to 14 mS cm−1 for amorphous Li3ScCl6. With a low activation energy of 0.18 eV, amorphous Li3ScCl6 is predicted to be among the most conductive amorphous halide electrolytes. To rationalize the composition-dependent transport, we identify two descriptors: the Li+ vibrational density of states (VDOS) center, which correlates inversely with diffusivity, and the average number of correlated bodies in string-like Li+ motion. Compositions in which Li+ has a lower VDOS center and migrates more by individual hopping rather than by concerted motion exhibit higher Li-ion diffusivities. These results suggest rich Li-ion transport characteristics in amorphous halide SSEs.
Related
- Visualizing surface-reaction-driven chloride migration and cascading failure in sulfide solid electrolytes
- Vacancy-enhanced Li solid-solution anodes for solid-state batteries: computational screening enabling high critical current density
- Computational Screening of Infrared Resonant Bands in Cholesterol Monohydrate for Selective Laser Lithotripsy of Cholesterol Gallstones
- Photon-pair characterization in an amorphous silicon waveguide
- Defect-stimulated amorphous track formation in SrTiO3 and KTaO3-application of analytical thermal spike model
BibTeX
@misc{liu2026computational,
title = {{Computational screening of amorphous lithium trivalent-metal chloride solid-state electrolytes}},
author = {Xiaolin Liu and Shuang and Xia and De-en Jiang},
howpublished = {arXiv},
year = {2026},
month = oct,
doi = {10.48550/arxiv.2610.34505},
eprint = {2610.34505},
archivePrefix = {arXiv},
url = {https://arxiv.org/abs/2610.34505},
}
RIS
TY - UNPB
TI - Computational screening of amorphous lithium trivalent-metal chloride solid-state electrolytes
AU - Xiaolin Liu
AU - Shuang
AU - Xia
AU - De-en Jiang
PY - 2026
DA - 2026/10/25
PB - arXiv
DO - 10.48550/arxiv.2610.34505
UR - https://arxiv.org/abs/2610.34505
AB - Amorphous solid-state electrolytes (SSEs) are attractive candidates for safe, high-energy-density all-solid-state batteries. The recent discovery that amorphous LiTaCl_6 and LiNbCl_6 reach room-temperature ionic conductivities above 10 mS cm^−1 with activation energies below 0.2 eV has spurred a broad search for new amorphous halide Li conductors. Here we report a computational screening of amorphous lithium trivalent-metal chlorides (Li-M(III)-Cl) using molecular dynamics driven by a universal machine-learning force field. For the sixteen Li-M(III)-Cl compositions spanning fifteen rare-earth elements and indium, all phases exhibit fast room-temperature Li^+ diffusion, with diffusivities of roughly $2−5 \times 10^{-7}$ cm^2 s^−1. After scaling the conductivity versus diffusivity relation to an experimental LiTaCl_6 reference, the estimated room-temperature conductivities range from 7.7 mS cm^−1 for amorphous Li_3InCl_6 to 14 mS cm^−1 for amorphous Li_3ScCl_6. With a low activation energy of 0.18 eV, amorphous Li_3ScCl_6 is predicted to be among the most conductive amorphous halide electrolytes. To rationalize the composition-dependent transport, we identify two descriptors: the Li^+ vibrational density of states (VDOS) center, which correlates inversely with diffusivity, and the average number of correlated bodies in string-like Li^+ motion. Compositions in which Li^+ has a lower VDOS center and migrates more by individual hopping rather than by concerted motion exhibit higher Li-ion diffusivities. These results suggest rich Li-ion transport characteristics in amorphous halide SSEs.
ER -