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The ternary strategy has proven to be an effective method for improving the efficiency of organic solar cells (OSCs). However, designing and selecting the third component still pose challenges. In this study, this issue is addressed by focusing on the PBDB‐T:Y18‐F binary system and introducing a new, strong luminescent, asymmetric small‐molecule acceptor (SMA) called L8‐CBIC‐Cl, which shares a similar skeleton with Y18‐F. The similarity in molecular framework facilitates good compatibility between the two acceptors, resulting in the formation of an alloy‐like acceptor phase. Furthermore, the norbornenyl‐modified end group in L8‐CBIC‐Cl contributes to its strong luminescent properties, which in turn leads to a low non‐radiative energy loss and a high open‐circuit voltage. Consequently, the PBDB‐T:L8‐CBIC‐Cl:Y18‐F based ternary devices realize a high power conversion efficiency (PCE) up to 17.01%, which is higher than PBDB‐T:Y18‐F device (14.49%). Importantly, L8‐CBIC‐Cl exhibits a good universality as a guest acceptor in other three binary systems (D18:Y6, D18:BTP‐eC9‐4F, and D18:L8‐BO). The D18:L8‐BO:L8‐CBIC‐Cl device shows an impressive efficiency of 19%. The work demonstrates that employing SMA with a high PLQY and better miscibility with host acceptor as the third component has a great potential for developing high‐efficiency ternary OSCs. [ABSTRACT FROM AUTHOR]

Fluorination of end groups has been a great success in developing efficient small molecule acceptors. However, this strategy has not been applied to the development of polymer acceptors. Here, a dihalogenated end group modified by fluorine and bromine atoms simultaneously, namely IC‐FBr, is first developed, then employed to construct a new polymer acceptor (named PYF‐T) for all‐polymer solar cells (all‐PSCs). In comparison with its non‐fluorinated counterpart (PY‐T), PYF‐T exhibits stronger and red‐shifted absorption spectra, stronger molecular packing and higher electron mobility. Meanwhile, the fluorination on the end groups down‐shifts the energy levels of PYF‐T, which matches better with the donor polymer PM6, leading to efficient charge transfer and small voltage loss. As a result, an all‐PSC based on PM6:PYF‐T yields a higher power conversion efficiency (PCE) of 14.1% than that of PM6:PY‐T (11.1%), which is among the highest values for all‐PSCs reported to date. This work demonstrates the effectiveness of fluorination of end‐groups in designing high‐performance polymer acceptors, which paves the way toward developing more efficient and stable all‐PSCs. [ABSTRACT FROM AUTHOR]

The electron‐deficient A1 unit in A‐DA1D‐A structured acceptors is critical for optimizing the efficiency of organic solar cells (OSCs). Drawing inspiration from the high performance of the previously reported pyrido[2,3‐b]quinoxaline‐core acceptors, Py6, an isomer of Py1 is designed with a repositioned pyridine nitrogen atom, and further modified it by chlorinating Py6 to create Py7. Theoretical calculations show that chlorine incorporation strengthens intermolecular non‐covalent interactions and promotes the tighter molecular stacking, as confirmed by grazing‐incidence wide‐angle X‐ray scattering. Consequently, D18/Py7 device delivers the enhanced fill factor and short‐circuit current density, compared to D18/Py1 and D18/Py6 device. Notably, D18/Py7 device also yields a higher open‐circuit voltage of 0.871 V, significantly outperforming Py1 (0.764 V) and Py6 (0.723 V), due to the low nonradiative energy losses. Further studies reveal that introducing Cl directs hole density toward the central pyrido[3,4‐b]quinoxaline unit and decreases the charge transfer state ratio of D18/acceptor. This prompts triplet‐to‐singlet conversion and reduces non‐radiative recombination losses. Additionally, using a mutual donor–acceptor dilution strategy, the (D18:1wt.% Py7)/(Py7:1wt.% D18) device achieves an impressive efficiency of 19.60%. This work emphasizes the great potential of the Py‐series acceptors and demonstrates that chlorine incorporation effectively reduces non‐radiative losses. [ABSTRACT FROM AUTHOR]