Strain-activated light-induced halide segregation in mixed-halide perovskite solids

Light-induced halide segregation limits the bandgap tunability of mixed-halide perovskites for tandem photovoltaics. Here we report that light-induced halide segregation is strain-activated in MAPb(I 1−x Br x ) 3 with Br concentration below approximately 50%, while it is intrinsic for Br concentration over approximately 50%. Free-standing single crystals of CH 3 NH 3 Pb(I 0.65 Br 0.35 ) 3 (35%Br) do not show halide segregation until uniaxial pressure is applied. Besides, 35%Br single crystals grown on lattice-mismatched substrates (e.g. single-crystal CaF 2 ) show inhomogeneous segregation due to heterogenous strain distribution. Through scanning probe microscopy, the above findings are successfully translated to polycrystalline thin films. For 35%Br thin films, halide segregation selectively occurs at grain boundaries due to localized strain at the boundaries; yet for 65%Br films, halide segregation occurs in the whole layer. We close by demonstrating that only the strain-activated halide segregation (35%Br/45%Br thin films) could be suppressed if the strain is properly released via additives (e.g. KI) or ideal substrates (e.g. SiO 2 ). Mixed-halide perovskites are of interest for photovoltaic devices, but light-induced halide segregation obstructs bandgap tuning and is not fully understood. Here the authors study the effects of strain and iodide/bromide ratio on light-induced halide segregation in mixed-halide perovskites.