Brian Collins, Obaid Alqahtani, Maxime Babics, Julien Gorenflot, Victoria Savikhin, Thomas Ferron, Ahmed Balawi, Andreas Paulke, Zhipeng Kan, Michael Pope, Andrew Clulow, Jannic Wolf, Paul Burn, Ian Gentle, Dieter Neher, Michael Toney, Frédéric Laquai, Pierre Beaujuge
It is established that the nanomorphology plays an important role in performance of bulk-heterojunction (BHJ) organic solar cells. From intense research in polymer-fullerene systems, some trends are becoming apparent. For example, small ~10 nm domains, high crystallinity, and low miscibility are typically measured in high-performance systems. However, the generality of these concepts for small-molecule (SM) BHJs is unclear. We present a comprehensive study of performance, charge generation and extraction dynamics, and nanomorphology in SM-fullerene BHJ devices to probe these critical structure-property relationships in this class of materials. In the systems investigated, small domains remain important for performance. However, devices composed of highly mixed domains with modest crystallinity outperform those consisting of pure/highly crystalline domains. Such a result points to an alternative ideal morphology for SM-based devices that involves a predominant mixed phase. This stems from SM aggregation in highly mixed domains that both maximize interface for charge generation and establish continuous pathways for efficient charge extraction. Such a morphological paradigm should be considered in future SM systems in pursuit of high-efficiency large-scale solar power production.
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