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@ARTICLE{Ding:1037544,
author = {Ding, Jingxuan and Gupta, Mayanak K. and Rosenbach, Carolin
and Lin, Hung-Min and Osti, Naresh C. and Abernathy, Douglas
L. and Zeier, Wolfgang and Delaire, Olivier},
title = {{L}iquid-like dynamics in a solid-state lithium
electrolyte},
journal = {Nature physics},
volume = {21},
issn = {1745-2473},
address = {Basingstoke},
publisher = {Nature Publishing Group},
reportid = {FZJ-2025-00733},
pages = {118–125},
year = {2025},
abstract = {Superionic materials represent a regime intermediate
between the crystalline and liquid states of matter. Despite
the considerable interest in potential applications for
solid-state batteries or thermoelectric devices, it remains
unclear whether the fast ionic diffusion observed in
superionic materials reflects liquid-like dynamics or
whether the hops of mobile ions are inherently coupled to
more conventional lattice phonons. Here we reveal a
crossover from crystalline vibrations to relaxational
dynamics of ionic diffusion in the superionic compound
$Li_6PS_5Cl$, a candidate solid-state electrolyte. By
combining inelastic and quasi-elastic neutron-scattering
measurements with first-principles-based machine-learned
molecular dynamics simulations, we found that the
vibrational density of states in the superionic state
strongly deviates from the quadratic behaviour expected from
the Debye law of lattice dynamics. The superionic dynamics
emerges from overdamped phonon quasiparticles to give rise
to a linear density of states characteristic of
instantaneous normal modes in the liquid state. Further, we
showed that the coupling of lattice phonons with a dynamic
breathing of the $Li^+$ diffusion bottleneck enables an
order-of-magnitude increase in diffusivity. Thus, our
results shed insights into superionics for future energy
storage and conversion technologies.},
cin = {IMD-4},
ddc = {530},
cid = {I:(DE-Juel1)IMD-4-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001390246300001},
doi = {10.1038/s41567-024-02707-6},
url = {https://juser.fz-juelich.de/record/1037544},
}