Monolayer MnPS 3 Nanosheet Integration for Extended Exciton Diffusion and Charge Transport in High‐Performance Thickness‐Insensitive Organic Photovoltaics

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Abstract Industrial‐scale roll‐to‐roll processing of organic photovoltaics (OPVs) requires photoactive layers ≥300 nm for manufacturability and mechanical robustness, yet state‐of‐the‐art high‐efficiency systems remain confined to 80–120 nm due to intrinsic exciton diffusion and charge transport limitations. To resolve this fundamental thickness‐efficiency trade‐off, monolayer MnPS 3 nanosheet (1–2 nm) via liquid‐phase exfoliation are engineered to extend exciton diffusion lengths and out‐of‐plane charge mobility, as validated through multimodal characterization. The optimized PM6:Y6:MnPS 3 system achieves record efficiencies of 19.53% (100 nm) and 18.41% (300 nm), demonstrating unprecedented 94.3% thickness tolerance and setting the highest reported retention for thick‐film (>300 nm) OPVs. Universal applicability is evidenced through 20.45%/19.70% (D18‐Cl:L8‐BO system) and 20.41%/19.62% (D18:L8‐BO system) efficiencies at 100/300 nm, outperforming state‐of‐the‐art thick‐film devices. This monolayer MnPS 3 nanosheet integration paradigm establishes a general design rule for thickness‐insensitive organic semiconductors, overcoming the critical photon harvesting‐charge extraction dichotomy in industrial‐scale OPV manufacturing.

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