Hysteresis Analysis of Hole-Transport-Material-Free Monolithic Perovskite Solar Cells with Carbon Counter Electrode by Current Density–Voltage and Impedance Spectra Measurements

Due to the tremendous increase in power conversion efficiency (PCE) of organic–inorganic perovskite solar cells (PSCs), this technology has attracted much attention. Despite being the fastest-growing photovoltaic technology to date, bottlenecks such as current density–voltage (J–V) hysteresis have significantly limited further development. Current density measurements performed with different sweep scan speeds exhibit hysteresis and the photovoltaic parameters extracted from the current density–voltage measurements for both scan directions become questionable. A current density–voltage measurement protocol needs to be established which can be used to achieve reproducible results and to compare devices made in different laboratories. In this work, we report a hysteresis analysis of a hole-transport-material-free (HTM-free) carbon-counter-electrode-based PSC conducted by current density–voltage and impedance spectra measurements. The effect of sweep scan direction and time delay was examined on the J–V characteristics of the device. The hysteresis was observed to be strongly sweep scan direction and time delay dependent and decreased as the delay increased. The J–V analysis conducted in the reverse sweep scan direction at a lower sweep time delay of 0.2 s revealed very large increases in the short circuit current density and the power conversion efficiency of 57.7% and 56.1%, respectively, compared with the values obtained during the forward scan under the same conditions. Impedance spectroscopy (IS) investigations were carried out and the effects of sweep scan speed, time delay, and frequency were analyzed. The hysteresis was observed to be strongly sweep scan direction, sweep time delay, and frequency dependent. The correlation between J–V and IS data is provided. The wealth of photovoltaic and impendence spectroscopic data reported in this work on the hysteresis study of the HTM-free PSC may help in establishing a current density–voltage measurement protocol, identifying components and interfaces causing the hysteresis, and modeling of PSCs, eventually benefiting device performance and long-term stability.