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From small molecules to infinite superatomic sheetsDeveloping a precise understanding of structure-function relationships in molecular crystals canallow us to generate a wide range of properties from extremely simple building blocks. In the firsthalf of my talk, I will discuss how crystal engineering and defects affect the macroscopicproperties of amino acid crystals. Moreover, I will describe the molecular-level determination ofthe structure of defect sites, which are below the diffraction detection limit, using pyroelectricmeasurement coupled with dispersion-corrected density functional theory calculations andmolecular dynamics simulations.In the second half of my talk, I will introduce a new two-dimensional crystalline form of carbonthat we recently synthesized –– graphullerene. The constituent fullerene subunits in thesecrystals are arranged hexagonally in a covalently interconnected molecular sheet that can bemechanically exfoliated and characterized. I will describe how the properties of graphullerenediffer from those of graphene and molecular fullerenes.