Mesostructured Dodecagonal Quasicrystal: the Interplay Between Temperature Regulation and Kinetic Structural...

Quasicrystals, characterized by long-range order and the absence of translational symmetry, have attracted great attention due to their extraordinary physicochemical properties. Although quasicrystals have been discovered in various experimental systems, the formation mechanisms that yield quasicrystals at the mesostructural scale remain elusive. Herein, a unique formation pathway of dodecagonal quasicrystal in silica mesoporous crystals is reported, employing cationic surfactant as a soft template and organosilane as a co-structure directing agent. Diverse structures, namely, disordered, dodecagonal quasicrystals, A15, and two-dimensional (2D) hexagonal structures were obtained by increasing the reaction temperature. Time-interval experiments showed that the quasicrystal formation proceeded via a continuous structural transition from initially formed lamellar configurations to dodecagonal tiling. This phenomenon stands in contrast to the classic nucleation and growth mechanisms previously proposed. The formation of these structures is attributed to the interplay between thermodynamic and kinetic control factors, specifically the delicate balance of two opposing effects: a decrease in interfacial curvature due to elevated temperature and an increase in curvature induced by charge density matching at the interface between surfactant micelles and inorganic species. The findings provide fresh insights into the formation and structural regulation of soft matter quasicrystals.