Alkylated Indacenodithiophene-Based Non-fullerene Acceptors with Extended π-Conjugation for High-Performance Large-Area Organic Solar Cells

In this work, a series of A–D–A′–D–A-type electron acceptors based on alkylated indacenodithiophene (C8IDT), dicyanated thiophene-flanked 2,1,3-benzothiadiazole (CNDTBT), and 2-(3-oxo-2,3-dihydro-1H-inden-1-ylidene)malononitrile (INCN) or 2-(5,6-difluoro-3-oxo-2,3-dihydro-1H-inden-1-ylidene) malononitrile (FINCN) are synthesized in order to investigate the effect of substituents on their photovoltaic properties. The corresponding CNDTBT-C8IDT-INCN and CNDTBT-C8IDT-FINCN acceptors vary in their optical, electrochemical, morphological, and charge transport properties. The fluorinated-INCN-based acceptor (CNDTBT-C8IDT-FINCN) exhibits lower energy levels, improved absorptivity, narrower π–π spacing, and prominent fibrillar structures when it is blended with poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)-benzo[1,2-b:4,5-b′]dithiophene))-alt-5,5-(1′,3′-di-2-thienyl-5′,7′-bis(2-ethylhexyl)benzo [1′,2′-c:4′,5′-c′]dithiophene-4,8-dione)] (PBDB-T). CNDTBT-C8IDT-FINCN exhibits a high power conversion efficiency (PCE) of 12.33% due to its high and well-balanced charge carrier mobility and distinct face-on orientation. Furthermore, large-area organic solar cells (OSCs) (active area: 55.45 cm2) with CNDTBT-C8IDT-FINCN exhibit a high PCE of 9.21%. This result demonstrates that CNDTBT-C8IDT-FINCN is a suitable and promising electron acceptor for large-area OSCs.