Publication date: 15th December 2025
Bulk heterojunction (BHJ) organic solar cells have achieved high efficiencies but suffer from poor morphological stability due to phase separation after long-term operation. Single-component OSCs based on double-cable polymers, 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 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 show that fluorination strengthens non-covalent interactions, promoting well-aligned intermolecular donor–acceptor interfaces. These structurally and energetically ordered interfacial CTs enable ultrafast, efficient charge generation, establishing interfacial energetic modulation via fluorination as a powerful strategy for high-efficiency and stable organic photovoltaics.
J. Wu acknowledges the funding support from the National Natural Science Foundation of China (52303249), the Department of Science and Technology of Guangdong Province (2021QN02C110), the Guangzhou Municipal Science and Technology Bureau Projects (2024A04J4513). Authors also thank the Green e Materials Laboratory and the HKUST Materials Characterization and Preparation Facility (MCPF) Guangzhou (GZ) for their facilities and technical support. R.P., and J.R.D. acknowledge financial support from the UK EPSRC through the ATIP Programme Grant (EP/T028513/1) and the Plastic Electronics Centre for Doctoral Training (EP/L016702/1).
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