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Chen, Z., Chen, X., Qiu, B., Zhou, G., Jia, Z., Tao, W., Li, Y., Yang, YM., Zhu, H.
J Phys Chem Lett
Nonfullerene acceptors (NFAs) have attracted great attention in high-efficiency organic solar cells (OSCs). While the effect of molecular properties including structures and energetics on charge transfer has been extensively investigated, the effect of macroscopic-phase properties is yet to be revealed. Here we have performed a correlation study of the nanoscale-phase morphology on the photoexcited hole transfer (HT) process and photovoltaic performance by combining ultrafast spectroscopy with high temporal resolution and photo-induced force microscopy (PiFM) with high spatial and chemical resolution. In PM6/IT-4F, we observe biphasic HT behavior with a minor ultrafast (<100 fs) interfacial process and a major diffusion-mediated HT process until ∼100 ps, which depends strongly on phase segregation. Because of the interplay between charge transfer and transport, a compromised domain size of 20-30 nm for NFAs shows the best performance. This study highlights the critical role of phase morphology in high-efficiency OSCs.