This research employs inner side-chain engineering in C-shaped ortho-benzodipyrrole-based (CB) A-D-A non-fullerene acceptors (NFAs) CB8, CB12, CB16, and CB20, where side-chain configuration crucially influences self-assembly, single-crystal structures, and optoelectronic properties. The enthalpy of fusion at the melting point, combined with the intensity of the 730 nm solid-state absorption shoulder, suggests that the acceptor-acceptor (A-A) interactions follow the order: CB8 > CB12 > CB20 > CB16. Solution small- and wide-angle X-ray scattering (SWAXS) quantitatively reveals the successively increased donor-acceptor (D-A) association numbers of these CB derivatives with PM6, consistent with the reduction of their A-A self-assembly. Complementarily and comprehensively, transient absorption spectroscopy (TAS) shows a systematically shortened decay-time of charge transfer in the series of the binary PM6:CB (1:1.2 wt%) thin films, from 25.40 ps (CB8), to 16.13 ps (CB12), to 15.03 ps (CB20), and to 11.97 ps (CB16), following the increasing trend of CB-PM6 interaction strength. Correspondingly, the photovoltaic efficiency improves with the enhanced CB-PM6 interactions from PM6:CB8 (15.24%), to PM6:CB12 (16.66%), to PM6:CB20 (17.12%), and to PM6:CB16 (18.13%). These close correlations between the structures and photovoltaic properties elucidate the importance of minimizing A-A self-aggregation and enhancing D (PM6)-A (CBs) interactions via engineering the side chains in the CB-based acceptors.
- Side-Chains Engineered Self-Assembly of Ortho-Benzodipyrrole-Based Acceptors: Comprehensive Exploration of Structure-Interface-Photovoltaics Correlations
- Yung-Jing Xue - National Yang Ming Chiao Tung UniversityChen-Yu Chang - Natl Tsing Hua Univ, Dept Chem Engn, 101 Sec 2,Kuang Fu Rd, Hsinchu 300044, TaiwanChieh-Ming Hung - Theodore Roosevelt High SchoolChi-Chun Tseng - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, TaiwanJe-Wei Chang - National Synchrotron Radiation Research CenterChun-Jen Su - National Synchrotron Radiation Research CenterChia-Lin Tsai - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, TaiwanHan-Cheng Lu - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, TaiwanKuo-Hsiu Huang - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, TaiwanKuei-Yu Tai - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, TaiwanChien-Yi Ku - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, TaiwanChia-Shing Wu - Taiwan Space Agcy, 8F,9 Prosper 1st Rd,Hsinchu Sci Pk, Hsinchu 300, TaiwanSu-Ying Chien - Theodore Roosevelt High SchoolShang-Da Yang - National Tsing Hua University, College of Semiconductor ResearchBing-Huang Jiang - Ming Chi University of TechnologyChih-Ping Chen - Ming Chi University of TechnologyPi-Tai Chou - National Taiwan UniversityU-Ser Jeng - National Tsing Hua University, Department of Chemical EngineeringYen-Ju Cheng - Natl Yang Ming Chiao Tung Univ, Dept Appl Chem, 1001 Univ Rd, Hsinchu 30010, Taiwan
- Wiley
- 17
- Ministry of Education, Taiwan 113-2221-E-A49 -001; 113-2113-M-A49 -015 -MY3 / National Science and Technology Council TPS 25A / National Science and Technology Council, Taiwan
- Journal article
- 01/12/2025
- Advanced functional materials, Vol.35(49), e04705
- English