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Abstract:

Although metal halide perovskite photovoltaics have shown an unprecedented rise in power conversion efficiency (PCE), they remain far from their theoretical PCE limit. Among the highest efficiencies to date are delivered when polycrystalline films are enhanced via “molecular passivation”, but this can introduce new instabilities, in particular under severe accelerated aging conditions (e.g., at 85 °C in the dark or under full spectrum simulated sunlight). Here, we utilize a benzylammonium bromide passivation treatment to improve device performance, achieving the champion stabilized power output (SPO) of 19.5 % in a p-i-n device architecture. We correlate the improved device performance with a significant increase in charge carrier diffusion lengths, mobilities, and lifetimes. Furthermore, treated devices maintain an increased performance during 120 h combined stressing under simulated full spectrum sunlight at 85 °C, indicating that enhancement from this passivation treatment is sustained under harsh accelerated aging conditions. This is a crucial step toward real-world operation-relevant passivation treatments.

Abstract:

Mixed tin‐lead halide perovskites are promising low‐bandgap absorbers for all‐perovskite tandem solar cells that offer higher efficiencies than single‐junction devices. A significant barrier to higher performance and stability is the ready oxidation of tin, commonly mitigated by various additives whose impact is still poorly understood for mixed tin‐lead perovskites. Here, the effects of the commonly used SnF2 additive are revealed for FA0.83Cs0.17SnxPb1−xI3 perovskites across the full compositional lead‐tin range and SnF2 percentages of 0.1–20% of precursor tin content. SnF2 addition causes a significant reduction in the background hole density associated with tin vacancies, yielding longer photoluminescence lifetimes, decreased energetic disorder, reduced Burstein–Moss shifts, and higher charge‐carrier mobilities. Such effects are optimized for SnF2 addition of 1%, while for 5% SnF2 and above, additional nonradiative recombination pathways begin to appear. It is further found that the addition of SnF2 reduces a tetragonal distortion in the perovskite structure deriving from the presence of tin vacancies that cause strain, particularly for high tin content. The optical phonon response associated with inorganic lattice vibrations is further explored, exhibiting a shift to higher frequency and significant broadening with increasing tin fraction, in accordance with lower effective atomic metal masses and shorter phonon lifetimes.