Engineering Ultrasoft Interactions in Stiff All-DNA Dendrimers by Site-Specific Control of Scaffold Flexibility
- Author(s)
- Nataša Adžić, Clemens Jochum, Christos N. Likos, Emmanuel Stiakakis
- Abstract
A combined experimental and theoretical study of the structural correlations in moderately concentrated suspensions of all-DNA dendrimers of the second generation (G2) with controlled scaffold rigidity is reported here. Small-angle X-ray scattering experiments in concentrated aqueous saline solutions of stiff all-DNA G2 dendritic constructs reveal a novel anomalous liquid-like phase behavior which is reflected in the calculated structure factors as a two-step increase at low scattering wave vectors. By developing a new design strategy for adjusting the particle's internal flexibility based on site-selective incorporation of single-stranded DNA linkers into the dendritic scaffold, it is shown that this unconventional type of self-organization is strongly contingent on the dendrimer's stiffness. A comprehensive computer simulation study employing dendritic models with different levels of coarse-graining, and two theoretical approaches based on effective, pair-potential interactions, remarkably confirmed the origin of this unusual liquid-like behavior. The results demonstrate that the precise control of the internal structure of the dendritic scaffold conferred by the DNA can be potentially used to engineer a rich palette of novel ultrasoft interaction potentials that could offer a route for directed self-assembly of intriguing soft matter phases and experimental realizations of a host of unusual phenomena theoretically predicted for ultrasoft interacting systems.
- Organisation(s)
- Computational and Soft Matter Physics
- External organisation(s)
- Technische Universität Wien, University of Belgrade, Forschungszentrum Jülich
- Journal
- Small
- No. of pages
- 12
- ISSN
- 1613-6810
- DOI
- https://doi.org/10.1002/smll.202308763
- Publication date
- 2024
- Peer reviewed
- Yes
- Austrian Fields of Science 2012
- 103015 Condensed matter, 102009 Computer simulation
- Keywords
- ASJC Scopus subject areas
- Biotechnology, Chemistry(all), Biomaterials, Materials Science(all), Engineering (miscellaneous)
- Portal url
- https://ucris.univie.ac.at/portal/en/publications/engineering-ultrasoft-interactions-in-stiff-alldna-dendrimers-by-sitespecific-control-of-scaffold-flexibility(92a698f5-21c8-454c-9f34-695976bf123e).html