TY  - JOUR
AU  - Böger, Thorben
AU  - Strotmann, Kyra
AU  - Faka, Vasiliki
AU  - Maus, Oliver
AU  - Abernathy, Douglas L.
AU  - Granroth, Garrett E.
AU  - Jalarvo, Niina H.
AU  - Li, Cheng
AU  - Suard, Emmanuelle
AU  - Zeier, Wolfgang
TI  - Impact of structural coherence and disorder on the ionic transport and lattice dynamics in $Li^+$ -conducting argyrodites
JO  - Journal of materials chemistry / A
VL  - 13
SN  - 2050-7488
CY  - London ˜[u.a.]œ
PB  - RSC
M1  - FZJ-2025-04368
SP  - 39211-39228
PY  - 2025
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - 41132693
UR  - <Go to ISI:>//WOS:001599319000001
DO  - DOI:10.1039/D5TA07185B
UR  - https://juser.fz-juelich.de/record/1047538
ER  -