Influence of hydrophobic moieties on the crystallization of amphiphilic DNA nanostructures

DOI: 10.1063/5.0132484
Data DOI: 10.17863/CAM.92820

Authors: Michal Walczak (University of Cambridge) , Ryan A. Brady (King's College London) , Adrian Leathers (University of Cambridge) , Jurij Kotar (University of Cambridge) , Lorenzo Di Michele (University of Cambridge; Imperial College London)
Co-authored by industrial partner: No

Type: Journal Paper
Journal: The Journal Of Chemical Physics , VOL 158

State: Published (Approved)
Published: February 2023
Diamond Proposal Number(s): 24537 , 29072

Abstract: Three-dimensional crystalline frameworks with nanoscale periodicity are valuable for many emerging technologies, from nanophotonics to nanomedicine. DNA nanotechnology has emerged as a prime route for constructing these materials, with most approaches taking advantage of the structural rigidity and bond directionality programmable for DNA building blocks. Recently, we have introduced an alternative strategy reliant on flexible, amphiphilic DNA junctions dubbed C-stars, whose ability to crystallize is modulated by design parameters, such as nanostructure topology, conformation, rigidity, and size. While C-stars have been shown to form ordered phases with controllable lattice parameter, response to stimuli, and embedded functionalities, much of their vast design space remains unexplored. Here, we investigate the effect of changing the chemical nature of the hydrophobic modifications and the structure of the DNA motifs in the vicinity of these moieties. While similar design variations should strongly alter key properties of the hydrophobic interactions between C-stars, such as strength and valency, only limited differences in self-assembly behavior are observed. This finding suggests that long-range order in C-star crystals is likely imposed by structural features of the building block itself rather than the specific characteristics of the hydrophobic tags. Nonetheless, we find that altering the hydrophobic regions influences the ability of C-star crystals to uptake hydrophobic molecular cargoes, which we exemplify by studying the encapsulation of antibiotic penicillin V. Besides advancing our understanding of the principles governing the self-assembly of amphiphilic DNA building blocks, our observations thus open up new routes to chemically program the materials without affecting their structure.

Journal Keywords: Nanomedicine; Hydrophobic interactions; Antibiotics; Crystallization; DNA nanotechnology; Engineering science; Micelles; Cholesterol

Subject Areas: Chemistry, Medicine, Materials


Instruments: I22-Small angle scattering & Diffraction

Added On: 01/03/2023 10:26

Documents:
5.0132484.pdf

Discipline Tags:

Drug Delivery Physical Chemistry Health & Wellbeing Chemistry Materials Science Nanoscience/Nanotechnology Life Sciences & Biotech

Technical Tags:

Scattering Small Angle X-ray Scattering (SAXS)