Publication date: 15th December 2025
Printable organic solar cells are intrinsically interface‑rich: interfacial chemistry governs charge extraction, recombination, and durability, while optical design sets absorption and spectral selectivity. We develop a molecular “interface grammar” using self‑assembled monolayers (SAMs) to rationally control energetics and stability in non‑fullerene–acceptor OPVs. By tuning anchoring chemistry, conjugation, dipole orientation, and programmed SAM–BHJ interactions (π–π, quadrupolar), SAMs align work functions, improve wetting and molecular registry, suppress interdiffusion, and stabilize UV‑exposed contacts—enhancing carrier extraction, lowering non‑radiative losses, and extending operational stability [1]. Crucially, this same molecular logic is carried into manufacturing through azeotrope‑assisted SAM processing, which enables low‑temperature, printed p–i–n stacks with improved reproducibility and reduced solvent use—maintaining the interfacial benefits while meeting scalability and sustainability targets [2].
With robust OPV interfaces as the foundation, we then apply the identical SAM toolkit to the most fragile buried interface in perovskite/organic tandems: the interconnection layer (ICL), where imbalanced transport—especially inadequate hole transport in the organic subcell—causes voltage deficits and severe non‑radiative recombination. A hole‑transport SAM anchored to MoO3 converts its inherently n‑type character to a p‑type surface; a SAM/MoO3/SAM sandwich further strengthens hole extraction, balances carrier transport, and suppresses interfacial recombination, yielding tandems with 26.05% PCE and Voc = 2.21 V (certified 2.216 V) and improved stability [3]. Finally, we close the loop between chemistry and optics: high‑throughput transfer‑matrix simulations coupled to genetic algorithms co‑design the multilayer stack around these SAM‑engineered interfaces, optimizing absorption–parasitic trade‑offs and tailoring spectra for semitransparent and color‑tunable devices [4]. Together, SAM‑programmed interfaces, solvent‑lean scalable processing, and data‑guided optical co‑design form a coherent pathway from durable, high‑efficiency OPV to promising hybrid tandem cells
