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Hybrid lead halide perovskites (LHPs) are a class of semiconductor with novelproperties that are distinctively governed by structural fluctuations.Diffraction experiments sensitive to average, long-range order reveal a cubicstructure in the device-relevant, high-temperature phase. Local probes findadditional short-range order with lower symmetry that may govern thestructure-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 includinglong carrier lifetimes and facile halide migration. Here, we determine the truestructure of two prototypical hybrid LHPs, CH$_3$NH$_3$PbI$_3$ andCH$_3$NH$_3$PbBr$_3$, using a combination of single-crystal X-ray and neutrondiffuse scattering, neutron inelastic spectroscopy, and molecular dynamicssimulations. The remarkable collective dynamics we found are not suggested byprevious studies and consist of a network of local two-dimensional, circularpancake-like regions of dynamically tilting lead halide octahedra (lowersymmetry) that induce longer range intermolecular correlations within theCH$_3$NH$_3^+$ sublattice. The dynamic local structure can introduce transientferroelectric or antiferroelectric domains that increase charge carrierlifetimes, and strongly affect the halide migration, a poorly understooddegradation mechanism. Our approach of co-analyzing single-crystal X-ray andneutron diffuse scattering data with MD simulations will provide unparalleledinsights into the structure of hybrid materials and materials with engineereddisorder.

The nature of dynamic local order in CH$_3$NH$_3$PbI$_3$ and CH$_3$NH$_3$PbBr$_3$