Modulation of PEDOT:PSS pH for Efficient Inverted Perovskite Solar Cells with Reduced Potential Loss and Enhanced...

Inverted p-i-n perovskite solar cells (PVSCs) using PEDOT:PSS as the hole-transporting layer (HTL) is one of the most widely adopted device structures thus far due to its facile processability and good compatibility for high throughput manufacturing processes. However, most of the PEDOT:PSS-based CH₃NH₃PbI₃ PVSCs reported to date suffered an inferior open-circuit voltage (V_OC) (0.88-0.95 V) compared to that (1.05-1.12 V) obtained for common CH₃NH₃PbI₃ PVSCs, revealing a severe potential loss issue. Herein, we describe a simple method to alleviate this problem by tuning the pH value of PEDOT:PSS with a mild base, imidazole. Accompanied by the pH modulation, the blended imidazole concurrently tailors the surface texture and electronic properties of PEDOT:PSS to promote the quality and crystallization of the perovskite film deposited on top of it and enable better energy-level alignment at this corresponding interface. Consequently, the PVSC using this modified PEDOT:PSS HTL yields an enhanced power conversion efficiency (PCE) of 15.7% with an enlarged V_OC of 1.06 V and improved long-term stability. These outperform the pristine device showing a PCE of 12.7% with a much smaller V_OC of 0.88 V and unsatisfactory environmental stability.