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Photovoltaic conversion efficiency (PCE) of halide perovskite solar cells hasrisen spectacularly, yet the very crystalline structure of CH3NH3PbI3 remainsambiguous after extensive researches, and its polar nature remains hotlydebated. Here we present compelling evidences that CH3NH3PbI3 crystalsself-grown on FTO/TiO2 substrate consist of ferroic domains with alternatingpolar and nonpolar orders, in contrast to previous experimental and theoreticalexpectations, and polar domains possess reduced photocurrent. It is found thatpolar and nonpolar orders of CH3NH3PbI3 can be distinguished from theirdistinct lateral piezoresponse, energy dissipation, first and second harmonicelectromechanical couplings, and temperature variation, even though theirdifference in crystalline lattice is very subtle, and they possess two-waymemory effect through cubic-tetragonal phase transition. These findings resolvekey questions regarding polar nature of CH3NH3PbI3 and its implication onphotovoltaics, reconcile contradictory data widely reported, and point adirection toward engineering ferroic domains for enhanced PCE.

Ferroic Domains of Alternating Polar and Nonpolar Orders Regulate  Photocurrent in Single Crystalline CH3NH3PbI3 Films Self-grown on FTO/TiO2  Substrate