Despite their multifaceted advantages, inverted perovskite
solar
cells (PSCs) still suffer from lower power conversion efficiencies
(PCEs) than their regular counterparts, which is largely due to recombination
energy losses (E
loss) that arise from
the chemical, physical, and energy level mismatches, especially at
the interfaces between perovskites and fullerene electron transport
layers (ETLs). To address this problem, we herein introduce an aminium
iodide derivative of a buckybowl (aminocorannulene) that is molecularly
layered at the perovskite–ETL interface. Strikingly, besides
passivating the PbI2-rich perovskite surface, the aminocorannulene
enforces a vertical dipole and enhances the surface n-type character
that is more compatible with the ETL, thus boosting the electron extraction
and transport dynamics and suppressing interfacial E
loss. As a result, the champion PSC achieves an excellent
PCE of over 22%, which is superior compared to that of the control
device (∼20%). Furthermore, the device stability is significantly
enhanced, owing to a lock-and-key-like grip on the mobile iodides
by the buckybowls and the resultant increase of the interfacial ion-migration
barrier. This work highlights the potential of buckybowls for the
multifunctional surface engineering of perovskite toward high-performance
and stable PSCs.