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Calculation aided miscibility manipulation enables highly efficient polythiophene:nonfullerene photovoltaic cells

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Abstract

Polythiophenes, with merits of low cost and high scalability of synthesis, have received growing interest in organic solar cells. To date, the best-performing polythiophene:nonfullerene solar cells exhibit typical power conversion efficiencies (PCEs) of 10%–12%, which is much lower than those employing PM6- and D18-type polymers. This inferior performance is mostly limited by the improper miscibility between polythiophene and acceptors. Efforts on engineering the molecular structure to systematically tune the miscibility are required. With the aid of group contribution calculations, the miscibility of polythiophene:nonfullerene blend system was finely tuned by varying the ratios of siloxane-terminated chains and alkyl chains in ester-substituted polythiophenes through random copolymerization. Based on a series of the polythiophene and nonfullerene acceptors, the detailed analysis of blend miscibility and performance reveals a surprising anticorrelation between the Flory-Huggins interaction parameter (χaa) and the optimal time of solvent vapor annealing for device performance across these systems. Primarily due to the slightly higher χaa, the blend of PDCBT-Cl-Si5 and ITIC-Th1 results in a record-high PCE of 12.85% in polythiophene: nonfullerene solar cells. The results not only provide a calculation-guided approach for molecular design but also prove that precise control of the miscibility is an effective way to design high-performance polythiophene:nonfullerene blends and beyond.

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Acknowledgements

This work was supported by the National Natural Science Foundation of China (52073207, 22075200, 51703158, 51933008). L.Y. was also supported by the Peiyang Scholar Program of Tianjin University and the Open Fund of the State Key Laboratory of Luminescent Materials and Devices (South China University of Technology, 2020-skllmd-11). M. L. thanks the Peiyang Young Junior Faculty Program of Tianjin University (2019XRG-0021) and Independent Innovation Fund of Tianjin University (2020XZC-0105). L.Y. acknowledges the merit beam-time (Proposal ID: 15692) approved by Australian Synchrotron. GIWAXS characterizations by N.K. were performed on the SAXS/WAXS beamline at the Australian Synchrotron, part of ANSTO. Dr. Xuechen Jiao (Monash University) was appreciated for the kind help in GIWAXS data analysis.

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Authors and Affiliations

  1. Joint School of National University of Singapore and Tianjin University, International Campus of Tianjin University, Fuzhou, 350207, China

    Qi Wang & Yanhou Geng

  2. School of Materials Science and Engineering, Tianjin University, Tianjin, 300072, China

    Qi Wang, Miaomiao Li, Zhongxiang Peng, Yunfeng Deng, Long Ye & Yanhou Geng

  3. Tianjin Key Laboratory of Molecular Optoelectronic Science, Tianjin University, Collaborative Innovation Center of Chemical Science and Engineering (Tianjin), Tianjin, 300072, China

    Miaomiao Li, Yunfeng Deng, Long Ye & Yanhou Geng

  4. Australian Synchrotron, Clayton, Victoria, 3168, Australia

    Nigel Kirby

  5. State Key Laboratory of Luminescent Materials and Devices, South China University of Technology, Guangzhou, 510640, China

    Long Ye

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  1. Qi Wang
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  2. Miaomiao Li
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  3. Zhongxiang Peng
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  4. Nigel Kirby
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  7. Yanhou Geng
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Correspondence to Miaomiao Li, Long Ye or Yanhou Geng.

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Wang, Q., Li, M., Peng, Z. et al. Calculation aided miscibility manipulation enables highly efficient polythiophene:nonfullerene photovoltaic cells. Sci. China Chem. 64, 478–487 (2021). https://doi.org/10.1007/s11426-020-9890-6

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  • DOI: https://doi.org/10.1007/s11426-020-9890-6

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