2D Crystal Engineering of Nanosheets Assembled from Helical Peptide Building Blocks.

The successful integration of 2D nanomaterials into functional devices hinges on developing fabrication methods that afford hierarchical control across length-scales of the entire assembly. Here, we demonstrate structural control over a class of crystalline 2D nanosheets assembled from collagen triple helices. By lengthening the triple helix unit via sequential additions of Pro-Hyp-Gly triads, we impart sub-angstrom tuning over the 2D lattice. These subtle changes influence the overall nanosheet size, which can be adjusted across the mesoscale size regime. The internal structure is observed via cryo-TEM with direct electron detection, which provides real-space high-resolution images, in which individual triple helices comprising the lattice can be clearly discerned. These results establish a general strategy for tuning the structural hierarchy of 2D nanomaterials that employ rigid, cylindrical structural units.

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