Abstract

The effective design and synthesis of novel small-molecule donors (SMDs) is extremely essential for the in-depth study of the scientific problems of bulk heterojunction morphology and the improvement of photovoltaic performance in organic solar cells (OSCs). Importantly, developing a series of donors with different conjugated central donor (D) units is a remarkable strategy to obtain high-performance donors. Herein, two acceptor-donor-donor-acceptor (A-D-D-A) type oligomeric donors 2DTBDT and 2DTBDT-2T with two dithieno[2,3-d:2′,3′-d']benzo[1,2-b:4,5-b']dithiophene (DTBDT) as D units, without and with bithiophene as the π bridge respectively are designed and synthesized successfully. The central linked-DTBDT unit can provide a larger conjugated plane and promote π electron delocalization, which can effectively improve π-π interactions between donors and regulate the crystallinity. And we found that the π bridge provided 2DTBDT-2T with 12.31% efficiency that is already a high efficiency in OSCs, whereas 2DTBDT with merely 3.63% efficiency, both with 2,2′-((2Z,2′Z)-((12,13-bis(2-ethylhexyl)-3,9-diundecyl-12,13-dihydro-[1,2,5]thiadiazolo[3,4-e]thieno[2,"3′’:4′,5′]thieno[2′,3′:4,5]pyrrolo[3,2-g]thieno[2′,3′:4,5]thieno[3,2-b]indole,10-diyl)bis(methanylylidene))bis(5,6-difluoro-3-oxo-2,3-dihydro-1H-indene-2,1-diylidene)) dimalononitrile (Y6) as the acceptor. We conjecture that the main reason for the different device performance may be ascribed to the different molecular stacking orientation of the oligomeric donors and morphology features of the donors:Y6 blend films. Compared to the predominant face-on orientation of the 2DTBDT neat film, the 2DTBDT-2T neat film performed a preferential edge-on orientation, which obtained a smoother surface, stronger crystallinity and more uniform phase separation in the 2DTBDT-2T:Y6 blend films with nanofiber structure, which delivered higher and more balanced carrier mobilities, the more efficient exciton dissociation and reduced biomolecule recombination, therefore obtaining better power conversion efficiencies (PCEs). We speculate that the transformation of molecular stacking orientation of oligomeric donors is possibly due to that π bridge extended and twisted the molecular structure of 2DTDBT-2T, resulting in an edge-on orientation relative to the substrate. These findings demonstrate that the single-bond-linked donor strategy is an alternative method to design the donors towards high-performance OSCs.

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