Abstract
Bulk heterojunction (BHJ) organic solar cells (OSCs) have achieved high efficiencies but suffer from poor morphological stability due to phase separation after long-term operation. Single-component OSCs (SCOSCs) based on double-cable polymers (DCP), offer improved stability through covalently linked donor and acceptor units. However, their efficiency remains limited by inefficient charge generation arising from extensive intermixed morphologies. Here, we report a fluorinated double-cable polymer, DCPY2-F, which achieves an outstanding efficiency of 14.8% with high short-circuit current density of 26.83 mA cm-2. Ultrafast pump-probe transient absorption spectroscopy reveals that fluorination of DCPY2 into DCPY2-F accelerates interfacial charge transfer and long-range charge separation dynamics. The pump-push-probe transient absorption spectroscopy and steady-state electroluminescence show that the faster interfacial charge transfer arises from a reduced reorganization energy and a correspondingly accelerated molecular reorganization process (2.5 ps vs. 0.8 ps). Despite comparable acceptor aggregate sizes with DCPY2, DCPY2-F also shows faster long-range charge separation dynamics, which we attribute to a narrower charge transfer states (CTs) energetic distribution. Molecular dynamics simulations further reveal that fluorination strengthens non-covalent interactions, promoting well-aligned intermolecular donor–acceptor interfaces. These structurally and energetically ordered interfacial CT states enable ultrafast and efficient charge generation. In corresponding binary blends, fluorination similarly enhances charge-transfer dynamics and photocurrent. These findings establish a unified fluorination strategy for accelerating charge generation dynamics in both SCOSCs and blends, and provide a mechanistic understanding for improving charge generation for high-performance single-component systems.
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Acknowledgements
The authors thank the Green e Materials Laboratory and the HKUST Materials Characterization and Preparation Facility (MCPF), Guangzhou (GZ), for their facilities and technical support. J.W. discloses support for the research of this work from the National Natural Science Foundation of China [52303249].
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Li, Y., Luo, Y., Hai, Y. et al. Ultrafast charge-generation dynamics through interfacial energetic modulation for high-performance single-component organic photovoltaics with 14.8% efficiency. Nat Commun (2026). https://doi.org/10.1038/s41467-026-72792-z
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DOI: https://doi.org/10.1038/s41467-026-72792-z
