journal article·2025-06Open access

Molecular Control of the Donor/Acceptor Interface Suppresses Charge Recombination Enabling High‐Efficiency Single‐Component Organic Solar Cells

Yao Li, Richard A. Pacalaj, Yongmin Luo, Keren Ai, Yulong Hai, Shijie Liang, Kezhou Fan, Aleksandr A. Sergeev, Ruijie Ma, Top Archie Dela Peña, Jolanda S. Müller, Zijing Jin, P Shakya Tuladhar, Tao Jia, Jiannong Wang, Gang Li, Kam Sing Wong, Weiwei Li, James R. Durrant, Jiaying Wu

Advanced Materials· Volume 37· Issue 23

Abstract

Abstract Single‐component organic solar cells based on double cable polymers have achieved remarkable performance, with DCPY2 reaching a high efficiency of over 13%. In this study, DCPY2 is further optimized with an efficiency of 13.85%, maintaining a high fill factor (FF) without compromising the short circuit current. Despite its intermixed morphology, DCPY2 shows a reduced recombination rate compared to their binary counterpart (PBDB‐T:Y‐O6). This slower recombination in DCPY2 is attributed to the reduced wavefunction overlap of delocalized charges, achieved by spatially separating the donor and acceptor units with an alkyl linker, thereby restricting the recombination pathways. Adding 1,8‐diiodooctane (DIO) into DCPY2 further reduced the recombination rate by facilitating acceptor aggregation, allowing free charges to become more delocalized. The DIO‐assisted aggregation in DCPY2 (5% DIO) is evidenced by an increased pseudo‐pure domain size of Y‐O6. Fine molecular control at the donor/acceptor interface in the double‐cable polymer achieves reduced non‐geminate recombination under efficient charge generation, increased mobility, and charge carrier lifetime, thereby achieving superior performance. Nevertheless, the FF is still limited by relatively low mobility compared to the blend, suggesting the potential for further mobility improvement through enhanced higher‐dimensional packing of the double‐cable material.
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Research context

OpenAlex topics: Organic Electronics and Photovoltaics · Conducting polymers and applications · Perovskite Materials and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Advanced Materials Thrust Function Hub The Hong Kong University of Science and Technology (Guangzhou) Nansha Guangzhou 511400 P. R. China

Department of Chemistry Centre for Processable Electronics Imperial College London White City Campus London W12 0BZ UK

Beijing Advanced Innovation Center for Soft Matter Science and Engineering & State Key Laboratory of Organic‐Inorganic Composites Beijing University of Chemical Technology Beijing 100029 P. R. China

School of Science Department of Physics Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong SAR 999077 P. R. China

Department of Electrical and Electronic Engineering Research Institute for Smart Energy (RISE) Photonic Research Institute (PRI) The Hong Kong Polytechnic University Hong Kong SAR 999077 P. R. China

Department of Physics Imperial College London London SW7 2AZ UK

School of Optoelectronic Engineering School of Mechanical Engineering Guangdong Polytechnic Normal University Guangzhou 510665 P. R. China

School of Engineering Department of Chemical and Biological Engineering Hong Kong University of Science and Technology Clear Water Bay Kowloon Hong Kong SAR 999077 P. R. China

Funding

National Natural Science Foundation of China · Engineering and Physical Sciences Research Council · Guangzhou Municipal Science and Technology Bureau · Guangdong Provincial Department of Science and Technology

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