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@ARTICLE{Xu:890166,
author = {Xu, Zhengwei and Zhao, Yicheng and Zhang, Jiyun and Chen,
Keqiu and Brabec, Christoph J. and Feng, Yexin},
title = {{P}hase diagram and stability of mixed-cation lead iodide
perovskites: {A} theory and experiment combined study},
journal = {Physical review materials},
volume = {4},
number = {9},
issn = {2475-9953},
address = {College Park, MD},
publisher = {APS},
reportid = {FZJ-2021-00755},
pages = {095401},
year = {2020},
abstract = {Alloying structurally similar perovskites to form
mixed-cation lead iodide perovskites, e.g.,
CsxFA(1−x)PbI3, MAxFA(1−x)PbI3, and
CsxMAyFA(1−x−y)PbI3, could improve the performance of
perovskite-based solar cells and light-emitting diodes.
However, a phase diagram of them and a clear understanding
of the underlying atomic-scale mechanism are still lacking.
Using ab initio calculations combined with high-throughput
experimentation, we demonstrate the phase diagram of
mixed-cation lead iodide perovskites. Only a small
proportion of monovalent cations (Cs+/Rb+/MA+) could be
incorporated into the FAPbI3/MAPbI3 matrix; otherwise it
will be separated into δ-CsPbI3, δ-RbPbI3, MAI, etc. The
smaller the radius of doping cations, the harder it is to
incorporate them into a perovskite lattice and the easier it
is to stabilize the perovskite phase. In FAPbI3-based
multication perovskites, moreover, over 10 mol $\%$ alloying
is needed to convert δ phase to α phase at room
temperature. The combined upper and lower limits for doping
concentration restrict the appropriate alloying ratio to a
narrow window. We further plot the relative energy diagram
for triple-cation perovskite CsxMAyFA(1−x−y)PbI3, which
reveals the ideal doping ratio for uniform stable alloying.
This theory-experiment-combined study provides a clear
microscopic picture of phase stability and segregation for
mixed-cation perovskite solids.},
cin = {IEK-11},
ddc = {530},
cid = {I:(DE-Juel1)IEK-11-20140314},
pnm = {121 - Solar cells of the next generation (POF3-121) / 540 -
Advanced Engineering Materials (POF3-500)},
pid = {G:(DE-HGF)POF3-121 / G:(DE-HGF)POF3-540},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000571166200001},
doi = {10.1103/PhysRevMaterials.4.095401},
url = {https://juser.fz-juelich.de/record/890166},
}