Enhancing molecular stacking and fiber morphology of biaxially conjugated acceptors via cyano substitution to achieve 19.71% efficiency in binary organic solar cells
摘要
Biaxially conjugated acceptors (BCAs) have emerged as a promising strategy for the design of high-performance organic solar cell materials, achieved through the incorporation of an additional conjugated core to enhance intermolecular interactions. Herein, we develop three BCAs (designated T1, T2, and T3), differentiated by the cyano group numbers in their central core. It is observed that Cyano substitution strengthens intermolecular interactions, leading to increased crystal coherence lengths. Notably, the D18:T2 blend exhibits pronounced fringed-micelle structures—a first in BCAs—wherein micelles are substantially larger than fibers, resulting in superior morphological characteristics. Consequently, the D18:T2 device attains a power conversion efficiency (PCE) of 19.05%, outperforming that of devices based on T1 and T3 due to improved exciton diffusion and charge transport. An incremental enhancement to a PCE of 19.71% is realized by substituting the PEDOT:PSS layer with a selfassembled 2PACz monolayer. Additionally, the T2-based device sustains efficiencies exceeding 17.5% across a broad thickness range of 120–300 nm, demonstrating low sensitivity to film thickness variations. This study not only confirms the crucial role of cyano substitution in elevating the efficiency of BCAs, but also illustrates how such groups strengthen molecular interactions, thereby facilitating the formation of fringed-micelle structures that positively impact the device efficiency.