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J Am Chem Soc. 2017 Jul 5;139(26):8915-8921. doi: 10.1021/jacs.7b02969. Epub 2017 Jun 21.

Water Dynamics from the Surface to the Interior of a Supramolecular Nanostructure.

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Department of Materials Science and Engineering, §Department of Chemistry, ⊥Department of Chemical and Biological Engineering, and∇Department of Biomedical Engineering, Northwestern University , Evanston, Illinois 60208, United States.
Department of Chemistry and Biochemistry, University of California , Santa Barbara, California 93106, United States.


Water within and surrounding the structure of a biological system adopts context-specific dynamics that mediate virtually all of the events involved in the inner workings of a cell. These events range from protein folding and molecular recognition to the formation of hierarchical structures. Water dynamics are mediated by the chemistry and geometry of interfaces where water and biomolecules meet. Here we investigate experimentally and computationally the translational dynamics of vicinal water molecules within the volume of a supramolecular peptide nanofiber measuring 6.7 nm in diameter. Using Overhauser dynamic nuclear polarization relaxometry, we show that drastic differences exist in water motion within a distance of about one nanometer from the surface, with rapid diffusion in the hydrophobic interior and immobilized water on the nanofiber surface. These results demonstrate that water associated with materials designed at the nanoscale is not simply a solvent, but rather an integral part of their structure and potential functions.


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