Abstract
The self-assembly of inorganic nanoparticles to larger structures is of great research interest as it allows the fabrication of novel materials with collective properties correlated to the nanoparticles’ individual characteristics. Recently developed methods for controlling nanoparticle organisation have enabled the fabrication of a range of new materials. Amongst these, the assembly of nanoparticles using DNA has attracted significant attention due to the highly selective recognition between complementary DNA strands, DNA nanostructure versatility, and ease of DNA chemical modification. In this review we discuss the application of various chemical DNA modifications and molecular intercalators as tools for the manipulation of DNA-nanoparticle structures. In detail, we discuss how DNA modifications and small molecule intercalators have been employed in the chemical and photochemical DNA ligation in nanostructures; DNA rotaxanes and catenanes associated with reconfigurable nanoparticle assemblies; and DNA backbone modifications including locked nucleic acids, peptide nucleic acids and borane nucleic acids, which affect the stability of nanostructures in complex environments. We conclude by highlighting the importance of maximising the synergy between the communities of DNA chemistry and nanoparticle self-assembly with the aim to enrich the library of tools available for the manipulation of nanostructures.
Highlights
There have been significant advancements in controlling the nanoscale features of materials with the aim of fabricating materials with desired properties.[1]
A key advantage of the Peptide nucleic acids (PNAs)–PNA assembly system was that stable hybridisation could be achieved using a recognition length of only few bases. Another feature of the PNA-based systems was that a single base mismatch was enough to prevent nanoparticles from assembling, whereas a partial assembly was still observed in the DNA–DNA system, suggesting that PNA-driven assemblies may be more selective in recognition of mismatches
DNA is a superior biopolymer that has been employed as a tool to assemble nanoparticles and larger nanostructures
Summary
There have been significant advancements in controlling the nanoscale features of materials with the aim of fabricating materials with desired properties.[1]. By mixing two batches of DNA functionalised nanoparticles with a complementary DNA target, a macroscopic amorphous aggregate was obtained.[50] In an alternative approach, Alivisatos and collaborators attached a discrete number of DNA strands to direct the assembly of gold nanoparticles into small oligomers of particles.[47,52,53,54] Both groups demonstrated the powerful concept that DNAcoated nanoparticles can be considered as ‘‘artificial atoms’’, which can assemble into a versatile range of larger structures with novel properties. Each voxel represents a defined building unit of 3D space, which can be empty or occupied; the valence and coordination of each individual voxel is determined by the frame’s geometry (e.g. tetrahedral, octahedral or cubic), which can bind to each other through hybridisation This allows the definition of a lattice symmetry and a lattice composition through the material voxel design and enables the rational assembly of 3D ordered nanomaterials from desired nano-objects for a broad range of applications.[78,79]. We will review DNA backbone modifications (e.g. locked nucleic acids, peptide nucleic acids, borane nucleic acids and phosphorothioate DNA) and their role in the stability of nanoparticle self-assemblies
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