A Hole-Selective Self-Assembled Monolayer for Both Efficient Perovskite and Organic Solar Cells

Self-assembled monolayers (SAMs) emerging as promising hole-selective layers (HSLs) are advantageous for facile processability, low cost, and minimal material consumption in the fabrication of both perovskite solar cells (PSCs) and organic solar cells (OSCs). However, owing to the different nature between perovskites and organic semiconductors, few SAMs were reported to effectively accommodate both PSCs and OSCs at the same time. In this regard, a universally applicable SAM that can accommodate both perovskites and organic semiconductors could be desirable for simplifying cell manufacturing, especially from an industrial perspective. In this work, we designed a SAM, TDPA-Cl by introducing chlorinated phenothiazine as the headgroup and linking with anchor phosphonic acid through a butyl chain. The resulting dense SAM was carefully characterized in terms of molecular bonding, surface morphology, and packing density, and its functions in OSCs and PSCs were discussed from the aspects of interactions with the absorber layer, energy level alignment, and charge-selective dipoles. The PM6:Y6-based OSCs with TDPA-Cl SAM as the HSL showed a superior performance to those with PEDOT:PSS. Furthermore, the universality was proved with an efficiency of 17.4% in the D18:Y6 system. In PSCs, the TDPA-Cl-based devices delivered a better performance of 22.4% than the PTAA-based devices (20.8%) with improved processability and reproducibility. This work represents a SAM with reasonably good compromise between the differing requirements of OSCs and PSCs. © 2024 American Chemical Society.