(353i) Advancing Efficiency and Stability of Perovskite Solar Cells through Rational Design of Hole Transport Layers and Passivating Ligands

Perovskite solar cells (PSCs) already rival silicon in power-conversion efficiency, yet interfacial losses and rapid degradation still impede commercialization. My doctoral research mitigates these hurdles through molecular engineering of (i) hole-transport layers (HTLs) and (ii) passivating surface ligands.

By integrating a recently reported pyrrole-functionalized 3,4-propylenedioxythiophene polymer (PPr) into the device stack, I demonstrated that improved energy alignment, defect healing, and surface hydrophobicity can be achieved without the cost and solubility penalties of conventional PEDOT derivatives. PPr-based PSCs reach 21.5 % efficiency and retain >95 % of their initial output after 4 000 h at 65 % RH.

I uncovered an overlooked loss pathway in aromatic passivators: low-lying ligand triplet states siphon photogenerated charges. Substituting pyrene with higher-triplet triphenylene (TP) suppresses this quenching channel, boosting efficiency from 23.1 % to 24.7 % and doubling photostability under continuous illumination.

Complementary contributions.

• One-step fluorinated passivation (F4TmI) couples 21.1 % efficiency with outstanding humidity and thermal robustness.
• Bidentate-ligand 2D perovskites deliver a record 25.3 % efficiency and extended operational lifetime.
• n-Doped poly(benzodifurandione) electrodes replace brittle TCOs, enabling flexible PSCs。
• Ternary-solvent blade coating yields large-area perovskite LEDs with >25 % EQE for biomedical NIR emitters.

Together, these advances show that targeted orbital tuning and interfacial design can simultaneously enhance efficiency, moisture tolerance, and photothermal durability in perovskite optoelectronics. In my AIChE presentation, I will detail how triplet-state management and HTL modification open a new stability frontier for PSC commercialization.