| Abstract
| - The structure of a novel molecularly ordered two-dimensional (2D) silicate framework in asurfactant-templated mesophase has been established by using a combination of solid-state nuclearmagnetic resonance (NMR) spectroscopy, X-ray diffraction, and quantum chemical and empirical force-field modeling. These materials are unusual in their combination of headgroup-directed 2D crystallineframework ordering, zeolite-like ring structures within the layers, and long-range mesoscopic organizationwithout three-dimensional (3D) atomic periodicity. The absence of registry between the silicate sheets,resulting from the liquidlike disorder of the alkyl surfactant chains, has presented significant challenges tothe determination of framework structures in these and similar materials lacking 3D crystalline order. Double-quantum 29Si NMR correlation experiments establish the interactions and connectivities between distinctintra-sheet silicon sites from which the structure of the molecularly ordered inorganic framework isdetermined.
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