Milled to order: toward predictive mechanochemistry of halide perovskites

Abstract

Mechanochemical milling is regarded as a scalable, solvent-free method that makes halide perovskites that solution processing cannot. Its deeper promise, though, is that mechanical force could become a new axis of synthetic control to turn milling from an empirical method into a predictive science. Halide perovskites are the ideal platform to establish this: their soft lattices and low formation energies make them intrinsically responsive to mechanical activation. Realising this requires settling what milling actually makes, and how: can a milled phase genuinely be trapped outside equilibrium, or is it just a convenient way to the equilibrium phase, and by what atomistic pathway does it work? These questions are mostly answered by assumption, while the in-situ and computational tools that resolved them for other material classes already exist. Closing this gap will unlock two design capabilities: mechanical energy used as a synthetic variable to tune phase selection, and metastability made programmable, producing trapped phases, specific intermediates, and compositions that have no possible solution route. Finally, two tests decide whether that control reaches practice: the state engineered during milling must survive into a working device, and the method must prove genuinely greener across the full device life cycle, rather than just solvent-free.