Abstract

<h2>Summary</h2> Surface energy of the underneath interlayer plays a crucial role in determining the morphology of bulk-heterojunction (BHJ) film in solution-processed organic solar cells (OSCs). However, little attention has been paid to this perspective at the microscopic level. In this study, we demonstrate an effective strategy to tune the nanoscale heterogeneous distribution of surface energy (HeD-SE) at interlayers through incorporating two-dimensional (2D) MoS<sub>2</sub> nanosheets, which modulate the component distribution, molecular orientation, and phase separation in the upper BHJ layers, leading to suppressed charge recombination and increased charge extraction in devices with enhanced power conversion efficiency (PCE) and device stability. Furthermore, we explore the relationship among the different surface energies of BHJs between the donor and the acceptor, the nanoscale HeD-SE at interlayers, and the PCEs of the resultant devices. This work reveals the impact of nanoscale heterogeneity in the distribution of surface energy in the underneath interlayers on the BHJ morphology and device performance in OSCs.

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