Assessing Effects of Different π bridges on Properties of Random Benzodithiophene-thienothiophene Donor and Non-fullerene Acceptor Based Active Layer

This report presents the effect of insertion of four different π bridges, furan, thienothiophene, thiophene, and thiazole, into a random benzodithiophene (BDT)-fluorinated-thienothiophene (TT-F) based donor. Starting from a structure of synthesized donor (D)-acceptor (A) random copolymer with 3:1 ratio, we have designed four D-π-A systems with four different π bridges. Structural, optoelectronic, and charge transport/transfer properties of these donors and donor/NDI (NDI = poly[N,N'-bis(2-hexyldecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5'-(2,2'-bithiophene)) blends are investigated using DFT and TD-DFT methodologies. Our results show that the thiazole based TzP1 oligomer has the deepest HOMO value resulting in the highest open circuit voltage among all systems. The maximum absorption wavelengths of π-linked systems are red-shifted compared to the parent molecule. Rates of charge transfer and charge recombination are the highest and smallest in case of the thiazole/NDI blend system. In addition, hole mobilities in thiophene, thienothiophene, and thiazole based systems are larger than in the parent system. The results indicate that the thiazole unit among the four π bridge units is the most suitable for active layer construction.