Two‐Dimensional Supramolecular Polymerization of DNA Amphiphiles is Driven by Sequence‐Dependent DNA‐Chromophore Interactions

Author:

Ghufran Rafique Muhammad1,Remington Jacob M.2,Clark Finley2,Bai Haochen1,Toader Violeta1,Perepichka Dmytro F.1,Li Jianing23,Sleiman Hanadi F.1ORCID

Affiliation:

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

3. Current address: Department of Medicinal Chemistry and Molecular Pharmacology Purdue University West Lafayette IN 47907 USA

Abstract

AbstractTwo‐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.

Funder

Canada Foundation for Innovation

National Institutes of Health

National Science Foundation

Publisher

Wiley

Subject

General Chemistry,Catalysis

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