DNA-Functionalized Supramolecular Polymers: Dynamic Multicomponent Assemblies with Emergent Properties

Abstract

Recent years have witnessed an increasing interest in hybrid molecular systems in which the programmability of DNA hybridization is used to introduce enhanced molecular control in synthetic systems. The first examples of DNA-functionalized supramolecular polymers have been reported only recently, but have already revealed structural and functional properties that are not easily obtained in either synthetic supramolecular polymers or DNA-only based systems. In this Topical Review, we provide an overview of the various forms of additional control offered by DNA hybridization for different types of supramolecular polymers and discuss how orthogonal supramolecular interactions in these hybrid systems can give rise to emergent structural and functional properties.

Supramolecular assembly of DNA-constructed vesicles

“…[8][9][10][11][12] Merging purely artificial DNA nucleotide surrogates with natural DNA nucleotides lead to DNA conjugates and the resulting functional supramolecular assemblies have recently gained much attention in the fields of nanotechnology and materials science. [13][14][15][16][17][18][19] Such functional supramolecular polymers feature properties beyond the classical role of DNA in biological systems, with applications in optoelectronic devices, drug delivery systems, and diagnostics to name a few. [20][21][22][23][24][25][26][27][28] However, vesicular morphologies are predominantly reported from lipid-DNA conjugates or DNA functionalized liposomes, [29][30][31][32][33][34] while the field apart from lipid-based DNA constructs remains largely unexplored.…”

Dynamic modulation of proximity-induced enzyme activity using supramolecular polymers

“…[10][11][12] Examples include the assembly of quasi-onedimensional fibrillar aggregates with tunable kinetic characteristics, hierarchical assemblies, and branched networks such as hydrogels and coacervates. [13][14][15] In addition, supramolecular polymers can be used as modular templates for the assembly of various biomolecules, including nanoparticles, 16,17 nucleic acids, 18,19 and proteins. [20][21][22][23] Recent work has revealed that intracellular signalling pathways heavily rely on the dynamic assembly of higher-order fibril-like aggregates that are structurally well-defined but open-ended and sometimes quasi-infinite.…”

DNA-inspired oligomers: from oligophosphates to functional materials

“…In particular, 1D assemblies of nucleic acids triggered widespread interest in the materials sciences for targeting functions beyond the obvious connection to biology. 23 For example, DNA can act as a versatile template for mineralization of various inorganic materials, providing access to nanoscale structures unattainable by other approaches. 24 The growth occurs via interactions of available negatively charged phosphate groups with suitable nucleation seeds followed by mineralization growth.…”