Wide‐Bandgap Perovskite Solar Cell Using a Fluoride‐Assisted Surface Gradient Passivation Strategy

Wide-band gap (1.68 eV) perovskite solar cells (PSCs) are important components of perovskite/Si tandem devices. However, the efficiency of wide band gap PSCs has been limited by their huge open-circuit voltage (Voc ) deficit due to non-radiative recombination. Deep-level acceptor defects are identified as the major killers of Voc , and they can be effectively improved by passivation with ammonium salts. Theoretical calculation predicts that increasing the distance between F and -NH3 + of fluorinated ammonium can dramatically enhance the electropositivity of -NH3 + terminals, thus providing strong adsorption onto the negatively charged IA and IPb anti-site defects. Characterizations further confirm that surface gradient passivation employing p-FPEAI demonstrates the most efficient passivation effect. Consequently, a record-efficiency of 21.63 % with the smallest Voc deficit of 441 mV is achieved for 1.68 eV-band gap inverted PSCs. Additionally, a flexible PSC and 1 cm2 opaque device also deliver the highest PCEs of 21.02 % and 19.31 %, respectively.