The stability of organic solar cells (OSCs) is an urgent problem for commercialization. In this work, a novel asymmetric molecule TB-4Cl was designed and synthesized. Quantum chemical computations revealed that TB-4Cl has a larger dipole moment of 1.98 Debye than that of Y6, which can induce a stronger intermolecular interaction. Without thermal annealing, devices based on PM6:TB-4Cl achieved a higher efficiency of 14.67%. Impressively, all of the devices showed a negligible difference in power conversion efficiency (PCE) before and after thermal-annealing treatment. Compared to the unencapsulated PM6:Y6-based devices, PM6:TB-4Cl-based devices exhibited improved thermal and air stability, evidenced by retaining around 75% (TB-4Cl) and 60% (Y6) after being heated at 100 °C in nitrogen for 110 h and 65% (TB-4Cl) and 50% (Y6) in air for 92 h. This work indicates that an A-DA'D-A asymmetric molecule can be a promising candidate for achieving stable OSCs with high efficiency.
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