Abstract
Chiral‐selective self‐assembly has markedly advanced the development of chiral materials. While the Sergeant and Soldiers principle allows for chirality amplification, it necessitates precise shape‐matching between chiral and achiral molecules, leading to a low chirality transfer efficiency—where one chiral molecule influences the chirality of a limited number of achiral molecules. Here, we show that this efficiency can be markedly enhanced by introducing chiral dimeric molecules. In this work, a single chiral molecule can control the chirality of up to 200 achiral molecules and even direct the assembly of inorganic nanoparticles into chiral nanocomposites through a sequential chirality transfer process. Moreover, this approach exhibits remarkable robustness, operating effectively without necessitating a precise match between chiral and achiral molecules. Consequently, using the same chiral molecules at an exceptionally low molar fraction (0.5 mol%) allows for the chiral‐selective assembly of achiral molecules over a broad spectrum, regardless of their packing habits, thus facilitating the creation of otherwise inaccessible chiral materials with modulated chiroptical properties. Last but not least, even a trace amount of chiral molecules can enhance the elastic modulus of the self‐assembled nanocomposites by a factor of eight.
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