Publication date: 17th February 2025
Inverted perovskite solar cells (PSCs) have emerged as a promising alternative to conventional structures, offering advantages such as simplified fabrication and improved stability. However, commonly used electron transport layers (ETLs) in p-i-n devices, such as fullerene-based materials, suffer from stability issues and induce a highly defective perovskite/ETL interface, featuring trap-mediated non-radiative recombination, which adversely impacts both the efficiency and stability of the resulting solar cells. The introduction of organic spacer moieties at the perovskite/ETL with stabilization effects has been proposed as an effective strategy to mitigate surface-assisted recombination and increase the stability of the device.
However, conventional molecular passivators are electronically insulating, resulting in charge confinement with respect to the light-absorbing material, thus limiting their functionality. In this context, optimizing the electronic properties of the passivating layer material offers a promising approach to overcome performance limitations by enhancing charge transport to the ETL.
In this contribution, we present the results of an experimental and theoretical study concerning the introduction of electroactive spacer moieties at the interface between the perovskite absorber and fullerene-based ETLs in inverted PSCs. We employ ab-initio molecular dynamics and density functional theory to elucidate the experimental findings and to unveil the underlying mechanisms connected to the interfacial charge transfer and improved stability brought about by the electroactive spacers. The use of electroactive spacers as ETL in fullerene-free devices is also explored.
U.R. acknowledges the Swiss National Foundation (grant N. 200020_219440) and computational resources from the Swiss National Computing Centre CSCS. V.C. acknowledges computational resources from the Swiss National Computing Centre CSCS.
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