Real-Time Nanoscale Open-Circuit Voltage Dynamics of Perovskite Solar Cells

Hybrid organic–inorganic perovskites based on methylammonium lead (MAPbI₃) are an emerging material with great potential for high-performance and low-cost photovoltaics. However, for perovskites to become a competitive and reliable solar cell technology their instability and spatial variation must be understood and controlled. While the macroscopic characterization of the devices as a function of time is very informative, a nanoscale identification of their real-time local optoelectronic response is still missing. Here, we implement a four-dimensional imaging method through illuminated heterodyne Kelvin probe force microscopy to spatially (<50 nm) and temporally (16 s/scan) resolve the voltage of perovskite solar cells in a low relative humidity environment. Local open-circuit voltage (V_oc) images show nanoscale sites with voltage variation >300 mV under 1-sun illumination. Surprisingly, regions of voltage that relax in seconds and after several minutes consistently coexist. Time-dependent changes of the local V_oc are likely due to intragrain ion migration and are reversible at low injection level. These results show for the first time the real-time transient behavior of the V_oc in perovskite solar cells at the nanoscale. Understanding and controlling the light-induced electrical changes that affect device performance are critical to the further development of stable perovskite-based solar technologies.