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@ARTICLE{Bger:1047538,
author = {Böger, Thorben and Strotmann, Kyra and Faka, Vasiliki and
Maus, Oliver and Abernathy, Douglas L. and Granroth, Garrett
E. and Jalarvo, Niina H. and Li, Cheng and Suard, Emmanuelle
and Zeier, Wolfgang},
title = {{I}mpact of structural coherence and disorder on the ionic
transport and lattice dynamics in ${L}i^+$ -conducting
argyrodites},
journal = {Journal of materials chemistry / A},
volume = {13},
issn = {2050-7488},
address = {London [u.a.]},
publisher = {RSC},
reportid = {FZJ-2025-04368},
pages = {39211-39228},
year = {2025},
abstract = {Solid-state batteries offer improved safety and higher
energy density compared to conventional lithium-ion systems.
Among candidate solid electrolytes, lithium argyrodites
stand out for their exceptional ionic conductivity and
compositional flexibility. Recent studies have revealed
strongly anharmonic, liquid-like ion and lattice dynamics in
these materials, including the collapse of soft phonons
driven by $Li^+ $diffusion, which impacts both local
vibrations and thermal transport. Yet, the connection
between the local structure, phonon dynamics, and
macroscopic heat transport remains unresolved. In this work,
we employ post-synthesis processing to tune microstructural
parameters—such as crystallite size, strain, and coherence
length—in two model systems: $Li_{5.5}PS_{4.5}Cl_{1.5}$
and $Li_6PS_5Br$. We systematically examine how mechanical
treatments influence structural coherence, ion and lattice
dynamics, and thermal transport. To further probe the role
of structural disorder, we investigate bromide substitution
in $Li_6PS_5I$. Across all compounds, thermal transport
above 100 K is dominated by diffusons. At lower
temperatures, however, structural disorder is significantly
more effective than reduced coherence length at suppressing
phonon-gas-type transport, underscoring the crucial role of
the local structure. Together with a detailed analysis of
lithium-ion dynamics, these results provide new insights
into how structural coherence and disorder govern both
transport and vibrational properties in fast ionic
conductors.},
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},
pubmed = {41132693},
UT = {WOS:001599319000001},
doi = {10.1039/D5TA07185B},
url = {https://juser.fz-juelich.de/record/1047538},
}