Balancing the Pre-aggregation and Crystallization Kinetics Enables High Efficiency Slot-Die Coated Organic Solar Cells with Reduced Non-radiative Recombination losses

Slot-die coating being compatible with the roll-to-roll technique has been regarded as a promising tool for the upscaling manufacturing of organic solar cells (OSCs). However, there has been a significant gap between the efficiencies of the state-of-the-art spin-coated devices and the scalable processed devices. The active layer morphology is crucial to achieve high efficiency in OSCs, which depends on the conditions of film fabrication. To figure out and optimize the slot-die coating process, a deeper understanding of the film formation kinetics is important. Herein, in-situ measurements of the slot-die coating process based on PM7:IT4F system is demonstrated to illustrate the aggregation and crystallization evolution at varied die temperatures and substrate temperatures. OSCs with high power conversion efficiency of 13.2 % are achieved at 60 oC die temperature / 60 oC substrate temperature due to the improved exciton dissociation, charge transport and suppressed non-radiative charge recombination. The optimized morphology is attributed to the balanced polymer pre-aggregation and small molecule crystallization kinetics. The unsuitable die temperature leads to overlarge phase separation and consequently inefficient exciton dissociation while the improper substrate temperature results in weak crystallization and the following shrunken carrier lifetime with strong non-radiative combination. This work provides fundamental understandings on the correlations among processing methodology, solution pre-aggregation, morphology formation kinetics, device physics and device performance and affords guidance for the device optimization in scalable manufacturing.