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Abstract Metal halide perovskites based on formamidinium (FA), or FA‐rich compositions have shown great promise for high‐performance photovoltaics. A deeper understanding of the impact of ambient conditions (e.g., moisture, oxygen, and illumination) on the possible reactions of FA‐based perovskite films and their processing sensitivities has become critical for further advances toward commercialization. Herein, we investigate reactions that take place on the surface of the FA_0.7Cs_0.3, mixed Br/I wide bandgap perovskite thin films in the presence of humid air and ambient illumination. The treatment forms a surface layer containing O, OH, and N‐based anions. We propose the latter originates from formamidine trapped at the perovskite/oxide interface reacting further to cyanide and/or formamidinate—an understudied class of pseudohalides that bind to Pb. Optimized treatment conditions improve photoluminescence quantum yield owing to both reduced surface recombination velocity and increased bulk carrier lifetime. The corresponding perovskite solar cells also exhibit improved performance. Identifying these reactions opens possibilities for better utilizing cyanide and amidinate ligands, species that may be expected during vapor processing of FA‐based perovskites. Our work also provides new insights into the self‐healing or self‐passivating of MA‐free perovskite compositions where FA and iodide damage could be partially offset by advantageous reaction byproducts. image 

Although C₆₀is usually the electron transport layer (ETL) in inverted perovskite solar cells, its molecular nature of C₆₀leads to weak interfaces that lead to non-ideal interfacial electronic and mechanical degradation. Here, we synthesized an ionic salt from C₆₀, 4-(1',5′-dihydro-1'-methyl-2'H-[5,6] fullereno-C₆₀-I_h-[1,9-c]pyrrol-2'-yl) phenylmethanaminium chloride (CPMAC), and used it as the electron shuttle in inverted PSCs. The CH₂-NH₃⁺head group in the CPMA cation improved the ETL interface and the ionic nature enhanced the packing, leading to ~3-fold increase in the interfacial toughness compared to C₆₀. Using CPMAC, we obtained ~26% power conversion efficiencies (PCEs) with ~2% degradation after 2,100 hours of 1-sun operation at 65°C. For minimodules (four subcells, 6 centimeters square), we achieved the PCE of ~23% with <9% degradation after 2,200 hours of operation at 55°C. 

We report on an examination of mobile ion concentration (N₀) in perovskite solar cells (PSCs) as a function of temperature and device architecture. 

Mechanical failure and chemical degradation of device heterointerfaces can strongly influence the long-term stability of perovskite solar cells (PSCs) under thermal cycling and damp heat conditions. We report chirality-mediated interfaces based onR-/S-methylbenzyl-ammonium between the perovskite absorber and electron-transport layer to create an elastic yet strong heterointerface with increased mechanical reliability. This interface harnesses enantiomer-controlled entropy to enhance tolerance to thermal cycling–induced fatigue and material degradation, and a heterochiral arrangement of organic cations leads to closer packing of benzene rings, which enhances chemical stability and charge transfer. The encapsulated PSCs showed retentions of 92% of power-conversion efficiency under a thermal cycling test (−40°C to 85°C; 200 cycles over 1200 hours) and 92% under a damp heat test (85% relative humidity; 85°C; 600 hours).