Combined <i>in Situ</i> Photoluminescence and X-ray Scattering Reveals Defect Formation in Lead-Halide Perovskite Films

Abstract

Lead-halide perovskites have established a firm foothold in photovoltaics and optoelectronics due to their steadily increasing power conversion efficiencies approaching conventional inorganic single-crystal semiconductors. However, further performance improvement requires reducing defect-assisted, nonradiative recombination of charge carriers in the perovskite layers. A deeper understanding of perovskite formation and associated process control is a prerequisite for effective defect reduction. In this study, we analyze the crystallization kinetics of the lead-halide perovskite MAPbI_3-<i>x</i>Cl_<i>x</i> during thermal annealing, employing <i>in situ</i> photoluminescence (PL) spectroscopy complemented by lab-based grazing-incidence wide-angle X-ray scattering (GIWAXS). <i>In situ</i> GIWAXS measurements are used to quantify the transition from a crystalline precursor to the perovskite structure. We show that the nonmonotonous character of PL intensity development reflects the perovskite phase volume, as well as the occurrence of the defects states at the perovskite layer surface and grain boundaries. The combined characterization approach enables easy determination of defect kinetics during perovskite formation in real-time.