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Emergent rhombus tilings from molecular interactions with M-fold rotational symmetry
S. Whitelam, I. Tamblyn, J.P. Garrahan, and P.H. Beton Physical Review Letters, 114, 115702 (2015) Understanding how molecules with specific rotational symmetries spontaneously organize into ordered network structures is central to engineering functional nanomaterials. In this work, we demonstrate that model molecules with particular rotational symmetries can self-assemble into network structures equivalent to rhombus tilings. Notably, this assembly occurs through an emergent process where molecules spontaneously select irregular 4-fold local coordination from a larger set of possible local binding geometries, rather than being explicitly programmed to do so. While simple geometry can rationalize why these network structures could exist, we show they form spontaneously only under specific dynamic conditions. We further identify that in certain regimes of parameter space, these rhombus tilings can reconfigure into triangular tilings, indicating structural flexibility depending on environmental conditions. This work reveals an important distinction between geometric possibility and dynamic self-assembly, with implications for the design of self-organizing molecular networks. (Cover Article) |
