Modification of Hydrophobic Self‐Assembled Monolayers with Nanoparticles for Improved Wettability and Enhanced Carrier Lifetimes Over Large Areas in Perovskite Solar Cells

The development of perovskite solar cells (PSCs) with low recombination losses at low processing temperatures is an area of growing research interest as it enables compatibility with roll‐to‐roll processing on flexible substrates as well as with tandem solar cells. The inverted or p–i–n device architecture has emerged as the most promising PSC configuration due to the possibility of using low‐temperature processable organic hole‐transport layers and more recently, self‐assembled monolayers such as [4‐(3,6‐dimethyl‐9 H ‐carbazol‐9‐yl)butyl]phosphonic acid (Me‐4PACz). However, devices incorporating these interlayers suffer from poor wettability of the precursor leading to pin hole formation and poor device yield. Herein, the use of alumina nanoparticles (Al 2 O 3 nanoparticles (NPs)) for pinning the perovskite precursor on Me‐4PACz is demonstrated, thereby improving the device yield. While similar wettability enhancements can also be achieved by using poly[(9,9‐bis(3′‐(( N , N ‐dimethyl)‐ N ‐ethylammonium)‐propyl)‐2,7‐fluorene)‐alt‐2,7‐(9,9‐dioctylfluorene)]dibromide (PFN‐Br), a widely employed surface modifier, the incorporation of Al 2 O 3 NPs results in significantly enhanced Shockley–Read–Hall recombination lifetimes exceeding 3 μs, which is higher than those on films coated directly on Me‐4PACz and on PFN‐Br‐modified Me‐4PACz. This translates to a champion power conversion efficiency of 19.9% for PSCs fabricated on Me‐4PACz modified with Al 2 O 3 , which is a ≈20% improvement compared to the champion device fabricated on PFN‐Br‐modified Me‐4PACz.