End-Group Engineering of Chlorine-Trialkylsiylthienyl Chain-Substituted Small-Molecule Donors for High-Efficiency...

Ternary architecture has been widely demonstrated as a facile and efficient strategy to boost the performance of organic solar cells (OSCs). However, the rational design of the third component with suitable core and end-group modification is still a challenge. Herein, two new small-molecule (SM) donors BT-CN and BT-ER, featuring the identical conjugated backbone with distinct end group, have been designed, synthesized, and introduced into the PM6:Y6 binary system as the second donor. Both molecules exhibit complementary absorption and good miscibility with PM6, contributing to the nanofibrous phases and strong face-on molecular packing. Importantly, the incorporation of BT-CN/BT-ER has significantly facilitated charge collection and transportation with remarkable suppression of carrier recombination. As a result, ternary OSCs with 20 wt% BT-CN/BT-ER achieved a PCE of 16.8%/17.22% with synchronously increased open-circuit voltage (V_OC ), short-circuit current density (J_SC ) and fill factor (FF). Moreover, replacing Y6 with L8-BO further improves the PCE to 18.05%/18.11%, indicating the universality of both molecules as the third component. This work demonstrates not only two efficient SM donors with 4,8-bis(4-chloro-5-(tripropylsilyl)thiophen-2-yl) benzo[1,2-b:4,5-b']dithiophene (BDTT-SiCl) as the core but also end group modification strategy to fine-tune the absorption spectrum, molecular packing, and energy levels of SM donors to construct high-performance ternary OSCs.