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Abstract Volatile solid additives have attracted increasing attention in optimizing the morphology and improving the performance of currently dominated non‐fullerene acceptor‐based organic solar cells (OSCs). However, the underlying principles governing the rational design of volatile solid additives remain elusive. Herein, a series of efficient volatile solid additives are successfully developed by the crossbreeding effect of chalcogenation and iodination for optimizing the morphology and improving the photovoltaic performances of OSCs. Five benzene derivatives of 1,4‐dimethoxybenzene (DOB), 1‐iodo‐4‐methoxybenzene (OIB), 1‐iodo‐4‐methylthiobenzene (SIB), 1,4‐dimethylthiobenzene (DSB) and 1,4‐diiodobenzene (DIB) are systematically studied, where the widely used DIB is used as the reference. The effect of chalcogenation and iodination on the overall property is comprehensively investigated, which indicates that the versatile functional groups provided various types of noncovalent interactions with the host materials for modulating the morphology. Among them, SIB with the combination of sulphuration and iodination enabled more appropriate interactions with the host blend, giving rise to a highly ordered molecular packing and more favorable morphology. As a result, the binary OSCs based on PM6:L8‐BO and PBTz‐F:L8‐BO as well as the ternary OSCs based on PBTz‐F:PM6:L8‐BO achieved impressive high PCEs of 18.87%, 18.81% and 19.68%, respectively, which are among the highest values for OSCs.
Zhou et al. (Mon,) studied this question.
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