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- W4319323474 abstract "Hybrid lead halide perovskites (LHPs) are a class of semiconductor with novel properties that are distinctively governed by structural fluctuations. Diffraction experiments sensitive to average, long-range order reveal a cubic structure in the device-relevant, high-temperature phase. Local probes find additional short-range order with lower symmetry that may govern the structure-function relationships of LHPs. However, the dimensionality, participating atoms, and dynamics of this short-range order are unresolved, impeding our understanding of technologically relevant properties including long carrier lifetimes and facile halide migration. Here, we determine the true structure of two prototypical hybrid LHPs, CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$, using a combination of single-crystal X-ray and neutron diffuse scattering, neutron inelastic spectroscopy, and molecular dynamics simulations. The remarkable collective dynamics we found are not suggested by previous studies and consist of a network of local two-dimensional, circular pancake-like regions of dynamically tilting lead halide octahedra (lower symmetry) that induce longer range intermolecular correlations within the CH$_3$NH$_3^+$ sublattice. The dynamic local structure can introduce transient ferroelectric or antiferroelectric domains that increase charge carrier lifetimes, and strongly affect the halide migration, a poorly understood degradation mechanism. Our approach of co-analyzing single-crystal X-ray and neutron diffuse scattering data with MD simulations will provide unparalleled insights into the structure of hybrid materials and materials with engineered disorder." @default.
- W4319323474 created "2023-02-08" @default.
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- W4319323474 date "2023-02-03" @default.
- W4319323474 modified "2023-10-18" @default.
- W4319323474 title "The nature of dynamic local order in CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$" @default.
- W4319323474 doi "https://doi.org/10.48550/arxiv.2302.01559" @default.
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