Efficient triisopropylsilylethynyl-substituted benzo[1,2-b:4,5-b] dithiophene-based random terpolymers enable non-fullerene organic solar cells with enhanced efficiency

Recent work has highlighted the pivotal role of ternary random polymers in the development of efficient high-performance polymer donors for organic solar cells (OSCs) and most of these D -A copolymer donors are so far constituted of an equal proportion of D and A-units. In this contribution, we report series of PM6-based ternary random terpolymers with unequal D- and A-units, namely, PM-TIPS10, PM-TIPS20 and PM-TIPS20, respectively by adding the 10%, 20% and 30% of simple and low-cost triisopropylsilylethynyl-substituted benzo[1,2-b:4,5-b ']dithiophene (BDT-TIPS) unit as second donor (D1) unit in polymer backbone based on D1 -A -D2 - A molecular design. Ascribed from the structural similarity of the two building blocks in the terpolymer backbone, these polymers showed orderly molecular packing, broadened light absorption, and the face -on orientation of the active layer to facilitate charge transport. Additionally, the new polymers displayed much deeper highest occupied molecular orbital (HOMO) energy levels than host PM6 polymer, which helped in enhancing the open circuit voltage (Voc) in the PM -TIPS -based OSCs. As a result, when combined with BTP-eC9 acceptor unit, PM-TIPS10 and PM-TIPS20 displayed best efficiency of 16.7 and 16.5% with a small energy loss of 0.484 and 0.473 eV, producing overall superior device parameters compared to PM6-based devices tested parallelly (PCE of 15.7%). This study reveals the corre- lation between introduction of the BDT-TIPS unit on polymer properties and photovoltaic performance and thus contributes to the design of high-PCE polymer donors by adapting a ternary random copolymerization strategy.