Manipulate Micrometer Surface and Nanometer Bulk Phase Separation Structures in the Active Layer of Organic Solar Cells via Synergy of Ultrasonic and High-Pressure Gas Spraying

For organic solar cells, the vertical and lateral micro-/nanometer-scale structure in the active layer largely determines the device performance. In this work, the surface and bulk domain size of the photoactive layer are successfully manipulated with a facile two-step spraying method, that is, an ultrathin active layer by high-pressure spraying is deliberately stacked on top of the thick active layer by ultrasonic spraying. Thus, the morphology is effectively optimized with the comprehensive study of optical and electrical characteristics, such as photon absorption, exciton dissociation efficiency, and bimolecular recombination. Moreover, the novel method can be used not only in the fullerene system but also in the nonfullerene system, demonstrating the remarkable universality through this synergy method. This work provides an easy and reliable strategy to improve photovoltaic device performance in the industrial large-area spray-coating process.