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Anions stabilize stacking of C5-symmetric macrocycles, called cyanostars, into dimers in solution and herein we demonstrate this stacking in solid-state crystals. We further show that this guest binding can be applied as a route to bilayer growth at the solution–graphite interface.

Graphical abstract: Anion-induced dimerization of 5-fold symmetric cyanostars in 3D crystalline solids and 2D self-assembled crystals

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