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Excellent conversion efficiencies of over 20 % and facile cell productionhave placed hybrid perovskites at the forefront of novel solar cell materialswith CH3NH3PbI3 being its archetypal compound. The question why CH3NH3PbI3 hassuch extraordinary characteristics, particularly a hugely efficient lightabsorption, is hotly debated with ferroelectricity being a promising candidate.This does, however, afford the crystal structure to be non-centrosymmetric andwe herein present crystallographic evidence as to how the symmetry breakingoccurs on a crystallographic, and therefore long-scale, level. While themolecular cation CH3NH3+ is intrinsically polar, it is heavily disordered andcannot be the sole reason for ferroelectricity. We show that it, nonetheless,plays an important role as it distorts the neighboring iodide positions fromtheir centrosymmetric positions.

Iodide-methylammonium interaction is responsible for ferroelectricity in CH3NH3PbI3