Abstract

AbstractOrganic single crystals with low defect density are key functional materials for next‐generation electronics. Classical crystallization commonly results in a high density of molecular steps, which are defects that can trap charge carriers and reduce the mobility of organic semiconductors. Herein, a novel nonclassical crystallization mechanism involving nucleation, fusion, and growth is designed. The introduction of the fusion stage changes the crystal growth mode from three‐dimensional island growth to two‐dimensional layer‐by‐layer growth and leads to large‐area two‐dimensional molecular crystals with almost no molecular steps. Therefore, the average mobility is observed to improve from 1.26 to 2.07 cm2 V−1 s−1. The nonclassical crystallization mechanism paves the way for atomically flat single crystals to probe the intrinsic optoelectronic properties of organic semiconductors.

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