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@ARTICLE{Till:907894,
author = {Till, Paul and Agne, Matthias and Kraft, Marvin A. and
Courty, Matthieu and Famprikis, Theodosios and Ghidiu,
Michael and Krauskopf, Thorben and Masquelier, Christian and
Zeier, Wolfgang G.},
title = {{T}wo-{D}imensional {S}ubstitution {S}eries
${N}a_3{P}_{1-x}{S}b_x{S}_{4-y}{S}e_y$: {B}eyond {S}tatic
{D}escription of {S}tructural {B}ottlenecks for ${N}a^{+}$
{T}ransport},
journal = {Chemistry of materials},
volume = {34},
number = {5},
issn = {0897-4756},
address = {Washington, DC},
publisher = {American Chemical Society},
reportid = {FZJ-2022-02273},
pages = {2410 - 2421},
year = {2022},
abstract = {Highly conductive solid electrolytes are fundamental for
all solid-state batteries with low inner cell resistance.
Such fast solid electrolytes are often found by systematic
substitution experiments in which one atom is exchanged for
another, and corresponding changes in ionic transport are
monitored. With this strategy, compositions with the most
promising transport properties can be identified fast and
reliably. However, the substitution of one element does not
only influence the crystal structure and diffusion channel
size (static) but also the underlying bonding interactions
and with it the vibrational properties of the lattice
(dynamic). Since both static and dynamic properties
influence the diffusion process, simple one-dimensional
substitution series only provide limited insights to the
importance of changes in the structure and lattice dynamics
for the transport properties. To overcome these limitations,
we make use of a two-dimensional substitution approach,
investigating and comparing the four single-substitution
series Na3P1–xSbxS4, Na3P1–xSbxSe4, Na3PS4–ySey, and
Na3SbS4–ySey. Specifically, we find that the diffusion
channel size represented by the distance between S/Se ions
cannot explain the observed changes of activation barriers
throughout the whole substitution system. Melting
temperatures and the herein newly defined anharmonic bulk
modulus─as descriptors for bonding interactions and
corresponding lattice dynamics─correlate well with the
activation barriers, highlighting the relevance of lattice
softness for the ion transport in this class of fast ion
conductors.},
cin = {IEK-12},
ddc = {540},
cid = {I:(DE-Juel1)IEK-12-20141217},
pnm = {1221 - Fundamentals and Materials (POF4-122)},
pid = {G:(DE-HGF)POF4-1221},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000812137700001},
doi = {10.1021/acs.chemmater.1c04445},
url = {https://juser.fz-juelich.de/record/907894},
}