Hysteresis and Its Correlation to Ionic Defects in Perovskite Solar Cells.

Ion migration has been reported to be one of the main reasons for hysteresis in the current-voltage (J-V) characteristics of perovskite solar cells. We investigate the interplay between ionic conduction and hysteresis types by studying Cs0.05(FA0.83MA0.17)0.95Pb(I0.9Br0.1)3 triple-cation perovskite solar cells through a combination of impedance spectroscopy (IS) and sweep-rate-dependent J-V curves. By comparing polycrystalline devices to single-crystal MAPbI3 devices, we separate two defects, ß and γ, both originating from long-range ionic conduction in the bulk. Defect ß is associated with a dielectric relaxation, while the migration of γ is influenced by the perovskite/hole transport layer interface. These conduction types are the causes of different types of hysteresis in J-V curves. The accumulation of ionic defects at the transport layer is the dominant cause for observing tunnel-diode-like characteristics in the J-V curves. By comparing devices with interface modifications at the electron and hole transport layers, we discuss the species and polarity of involved defects.

Single-Crystal Perovskite Solar Cells Exhibit Close to Half A Millimeter Electron-Diffusion Length.

Single-crystal halide perovskites exhibit photogenerated-carriers of high mobility and long lifetime, making them excellent candidates for applications demanding thick semiconductors, such as ionizing radiation detectors, nuclear batteries, and concentrated photovoltaics. However, charge collection depreciates with increasing thickness; therefore, tens to hundreds of volts of external bias is required to extract charges from a thick perovskite layer, leading to a considerable amount of dark current and fast degradation of perovskite absorbers. However, extending the carrier-diffusion length can mitigate many of the anticipated issues preventing the practical utilization of perovskites in the abovementioned applications. Here, single-crystal perovskite solar cells that are up to 400 times thicker than state-of-the-art perovskite polycrystalline films are fabricated, yet retain high charge-collection efficiency in the absence of an external bias. Cells with thicknesses of 110, 214, and 290 µm display power conversion efficiencies (PCEs) of 20.0, 18.4, and 14.7%, respectively. The remarkable persistence of high PCEs, despite the increase in thickness, is a result of a long electron-diffusion length in those cells, which was estimated, from the thickness-dependent short-circuit current, to be ≈0.45 mm under 1 sun illumination. These results pave the way for adapting perovskite devices to optoelectronic applications in which a thick active layer is essential.