Search

The hole‐transporting material (HTM), poly (3,4‐ethylene dioxythiophene) poly(styrene sulfonate) (PEDOT : PSS), is the most widely used material in the realization of high‐efficiency organic solar cells (OSCs). However, the stability of PEDOT : PSS‐based OSCs is quite poor, arising from its strong acidity and hygroscopicity. In addition, PEDOT : PSS has an absorption in the infrared region and high highest occupied molecular orbital (HOMO) energy level, thus limiting the enhancement of short‐circuit current density (Jsc) and open‐circuit voltage (Voc), respectively. Herein, two asymmetric self‐assembled molecules (SAMs), namely BrCz and BrBACz, were designed and synthesized as HTM in binary OSCs based on the well‐known system of PM6 : Y6, PM6 : eC9, PM6 : L8‐BO, and D18 : eC9. Compared with BrCz, BrBACz shows larger dipole moment, deeper work function and lower surface energy. Moreover, BrBACz not only enhances photon harvesting in the active layer, but also minimizes voltage losses as well as improves interface charge extraction/ transport. Consequently, the PM6 : eC9‐based binary OSC using BrBACz as HTM exhibits a champion efficiency of 19.70 % with a remarkable Jsc of 29.20 mA cm−2 and a Voc of 0.856 V, which is a record efficiency for binary OSCs so far. In addition, the unencapsulated device maintains 95.0 % of its original efficiency after 1,000 hours of storage at air ambient, indicating excellent long‐term stability. [ABSTRACT FROM AUTHOR]

The wearable application of flexible organic solar cells (f‐OSCs) necessitates high power conversion efficiency (PCE) and mechanical robustness. However, photoactive films based on efficient non‐fullerene small molecule acceptors (NF‐SMAs) are typically brittle, leading to poor mechanical stability in devices. In this study, we achieved a remarkable PCE of 18.06 % in f‐OSCs while maintaining ultrahigh mechanical robustness (with a crack‐onset strain (COS) of higher than 11 %) by incorporating a linker dimerized acceptor (DOY‐TVT). Compared to binary blends, ternary systems exhibit reduced non‐radiative recombination, suppressed crystallization and diffusion of NF‐SMAs, and improved load distribution across the chain networks, enabling the dissipation of the load energy. Thus, the ternary f‐OSCs developed in this study achieved, high PCE and stability, surpassing binary OSCs. Moreover, the developed f‐OSCs retained 97 % of the initial PCE even after 3000 bending cycles, indicating excellent mechanical stability (9.1 % higher than binary systems). Furthermore, the rigid device with inverted structure based on the optimal active layer exhibited a substantial increase in efficiency retention, with 89.6 % after 865 h at 85 °C and 93 % after more than 1300 h of shelf storage at 25 °C. These findings highlight the potential of the linker oligomer acceptor for realizing high‐performing f‐OSCs with ultrahigh mechanical robustness. [ABSTRACT FROM AUTHOR]