Dynamic nanodomains dictate macroscopic properties in lead halide perovskites

M Dubajic and JR Neilson and J Klarbring and X Liang and SA Bird and KC Rule and JE Auckett and TA Selby and G Tumen-Ulzii and Y Lu and YK Jung and C Chosy and ZM Wei and Y Boeije and MV Zimmermann and A Pusch and LL Gu and XG Jia and QY Wu and JC Trowbridge and EM Mozur and A Minelli and N Roth and KWP Orr and AM Soufiani and S Kahmann and I Kabakova and JN Ding and TM Wu and GJ Conibeer and SP Bremner and MP Nielsen and A Walsh and SD Stranks, NATURE NANOTECHNOLOGY, 20, 755-763 (2025).

DOI: 10.1038/s41565-025-01917-0

Lead halide perovskites have emerged as promising materials for solar energy conversion and X-ray detection owing to their remarkable optoelectronic properties. However, the microscopic origins of their superior performance remain unclear. Here we show that low-symmetry dynamic nanodomains present in the high-symmetry average cubic phases, whose characteristics are dictated by the A-site cation, govern the macroscopic behaviour. We combine X-ray diffuse scattering, inelastic neutron spectroscopy, hyperspectral photoluminescence microscopy and machine-learning-assisted molecular dynamics simulations to directly correlate local nanoscale dynamics with macroscopic optoelectronic response. Our approach reveals that methylammonium-based perovskites form densely packed, anisotropic dynamic nanodomains with out-of-phase octahedral tilting, whereas formamidinium-based systems develop sparse, isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. We demonstrate that these sparsely distributed isotropic nanodomains present in formamidinium-based systems reduce electronic dynamic disorder, resulting in a beneficial optoelectronic response, thereby enhancing the performance of formamidinium-based lead halide perovskite devices. By elucidating the influence of the A-site cation on local dynamic nanodomains, and consequently, on the macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics and X-ray imaging.

Return to Publications page