Publication date: 11th March 2026
Organic photovoltaic (OPV) devices have achieved high efficiency, but further progress is constrained by interfacial recombination and sub-optimal morphology, and limited stability. Here, we address these challenges by introducing CsPbI3 perovskite quantum dots (PQDs) as an interlayer at the D18/Y6 interface, deposited via an orthogonal-solvent layer-by-layer process. Incorporation of an optimized PQDs interlayer boosts the power conversion efficiency from 16.7% in the binary device to 18.8% in the ternary architecture, corresponding to a relative increase of ~12%. The systematic comparative study of morphology, optical/optoelectronic and electrical characteristics, as well as the related charge recombination and transfer dynamics, revealed that the D18/PQDsY6 assembly provided a unique electronic structure that passivates PQDs surface defects and mitigates interdiffusion of the organic layers, enabling improved microstructure regulation, leading to enhanced fill factor. Moreover, the high dielectric constant of the PQDs appears to facilitate exciton dissociation at the D18/Y6 interface, allowing the PQDs to act as a relay that separates and stabilizes charges at the D18/PQDs/Y6 junction, thereby reducing the trap-assisted recombination. This leads to suppressed non-radiative recombination losses, resulting in higher open-circuit voltage (VOC) and short-circuit current (JSC). Beyond performance gains, the PQDs interlayer also improves the shelf-life stability under N2, prolonging the stability for the pristine devices over 12 months. Hence, our findings demonstrate that introducing CsPbI₃ PQDs interlayer, implemented via orthogonal-solvent LBL processing, provides an effective route to tune interfacial morphology and energetics, offering a practical strategy to further enhance both efficiency and stability in OPV devices.
E. M. acknowledges the Iberdrola Foundation under Marie Skłodowska-Curie-MSCA-COFUND, funding from the European Union's Horizon 2020 research and innovation program, Grant Agreement No 101034297 for awarding the Energy for Future-E4F-postdoctoral individual fellowship program 2024-2025.
