Publication date: 22nd July 2026
Local atomic structure often differs from the global average structure as measured with diffraction and yet the local structure has a profound impact on materials functionalities. This structure-function relationship applies in many materials classes, ranging from organics to Li-ion battery cathodes to oxide and halide perovskites. Accurately characterizing this local structure has proven challenging but recent advances in neutron and X-ray diffuse scattering (“between” Bragg peaks) has enabled local structure determination.
In this talk, I will discuss the importance of local structure and how this can be quantified and will demonstrate this for organic-inorganic hybrid halide perovskites [1,2,3]. While the importance of lattice dynamics and dynamical (dis)order have been recognized in these materials, their nature is only poorly known and understood. We used X-ray and neutron diffuse scattering coupled with molecular dynamics to quantify the nature, size, and time scale associated with dynamical local order in CH3NH3PbI3 and CH3NH3PbBr3 perovskites [1] and on [(CHN2H4)xCs(1-x)]PbBr3 alloys. We observe that for CH3NH3 (MA or methylammonium) A-site cations the nominally cubic perovskite consists of dynamical, two-dimensional (2D) sheets of lower symmetry tetragonal regions of about three nm diameter with several picosecond lifetimes. For (CHN2H4)PbBr3, we observe elliptical, small (ca 3 nm) three dimensional (3D) tetragonal domains, consistent with recent work [2], while Cs has 2D sheet domains [3]. With increasing CHN2H4 (FA or formamidinium) on the A-site, creating [FACs]PbBr3 alloys, we observe a cross-over from the elliptical tetragonal domains to the 2D sheets near about 20% FA with a small region of co-existence. The implications on these dynamical local domains for halide perovskite properties will be discussed.
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