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We find significant differences between degradation and healing at thesurface or in the bulk for each of the different APbBr3 single crystals(A=CH3NH3+, methylammonium (MA); HC(NH2)2+, formamidinium (FA); and cesium,Cs+). Using 1- and 2-photon microscopy and photobleaching we conclude thatkinetics dominate the surface, and thermodynamics the bulk stability.Fluorescence-lifetime imaging microscopy, as well as results from several othermethods, relate the (damaged) state of the halide perovskite (HaP) afterphotobleaching to its modified optical and electronic properties. The A cationtype strongly influences both the kinetics and the thermodynamics of recoveryand degradation: FA heals best the bulk material with faster self-healing; Cs+protects the surface best, being the least volatile of the A cations andpossibly through O-passivation; MA passivates defects via methylamine fromphoto-dissociation, which binds to Pb2+. DFT simulations not only provideinsight into the latter conclusion, but also show the importance and stabilityof the Br3- defect. These results rationalize the use of mixed A-cationmaterials for optimizing both solar cell stability and overall performance ofHaP-based devices, and provide a basis for designing new HaP variants.

The pursuit of stability in halide perovskites: the monovalent cation and the key for surface and bulk self-repair