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Four {\pi}-extended phosphoniumfluorene electrolytes ({\pi}-PFEs) areintroduced as hole-blocking layers (HBL) in inverted architecture planarperovskite solar cells (PVSCs) with the structure ofITO/PEDOT:PSS/MAPbI3/PCBM/HBL/Ag. The deep-lying highest occupied molecularorbital (HOMO) energy level of the {\pi}-PFEs effectively blocks holes,decreasing contact recombination. We demonstrate that the incorporation of{\pi}-PFEs introduces a dipole moment at the PCBM/Ag interface, resulting in asignificant enhancement of the built-in potential of the device. Thisenhancement results in an increase in the open-circuit voltage of the device byup to 120 mV, when compared to the commonly used bathocuproine HBL. The resultsare confirmed both experimentally and by numerical simulation. Our workdemonstrates that interfacial engineering of the transport layer/contactinterface by small molecule electrolytes is a promising route to suppressnon-radiative recombination in perovskite devices and compensate for anon-ideal energetic alignment at the hole-transport layer/perovskite interface.

Enhancing the Open-Circuit Voltage of Perovskite Solar Cells by up to  120 mV using {\pi}-Extended Phosphoniumfluorene Electrolytes as Hole Blocking  Layers