Two-Dimensional Supramolecular Polymerization of DNA Amphiphiles is Driven by Sequence-Dependent DNA-Chromophore Interactions |
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| Authors: | Muhammad Ghufran Rafique Dr Jacob M Remington Finley Clark Haochen Bai Dr Violeta Toader Prof Dmytro F Perepichka Prof Jianing Li Prof Hanadi F Sleiman |
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| Institution: | 1. Department of Chemistry, McGill University, 801 Sherbrooke St W, H3A 0B8 Montréal, QC, Canada;2. Department of Chemistry, The University of Vermont, 05405 Burlington, VT, USA |
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| Abstract: | Two-dimensional (2D) assemblies of water-soluble block copolymers have been limited by a dearth of systematic studies that relate polymer structure to pathway mechanism and supramolecular morphology. Here, we employ sequence-defined triblock DNA amphiphiles for the supramolecular polymerization of free-standing DNA nanosheets in water. Our systematic modulation of amphiphile sequence shows the alkyl chain core forming a cell membrane-like structure and the distal π-stacking chromophore block folding back to interact with the hydrophilic DNA block on the nanosheet surface. This interaction is crucial to sheet formation, marked by a chiral “signature”, and sensitive to DNA sequence, where nanosheets form with a mixed sequence, but not with a homogeneous poly(thymine) sequence. This work opens the possibility of forming well-ordered, bilayer-like assemblies using a single DNA amphiphile for applications in cell sensing, nucleic acid therapeutic delivery and enzyme arrays. |
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| Keywords: | DNA Molecular Dynamics Simulations Nanosheets Self-Assembly Sequence-Controlled Polymers |
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