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Title: DNA-directed assembly of inorganic nanoparticles
Author: Harimech, Pascal
ISNI:       0000 0004 5990 6288
Awarding Body: University of Southampton
Current Institution: University of Southampton
Date of Award: 2016
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In the last two decades, inorganic nanoparticles have become an active field of research due to their unique physical properties. The advancements in the control over size, shape and composition opened up many potential applications in a wide range of fields from optoelectronics to medicine. A lot of research focusses on the controlled assembly of nanoparticles into larger pre-defined structures. A very successful approach uses DNA-functionalised nanoparticles as building blocks, which are capable of self-assembly driven by the DNA design. Such nanoparticle assemblies can infer new optical properties like circular dichroism or make multi-functional materials for advanced applications. In this work, a novel tool for the ligation of nanoparticle assemblies with DNA is presented. The UV-responsive molecule 3-cyanovinyl carbazole was embedded in DNA strands as a crosslinker for the covalent linkage of dsDNA. The covalent bond significantly increases the stability of dsDNA even in unfavourable conditions allowing a wider range of applicability. Unlike with other crosslinking techniques, already formed interstrand bonds can be reversed with UV-B light as an external stimulus. The efficient application of 3-cyanovinyl carbazole in tetrahedral gold nanoparticle assemblies is demonstrated for the first time. In addition, limitations of the strain-promoted azide-alkyne click reaction in the same system are revealed. DNA-directed hetero-assemblies consisting of CdSe/ZnS quantum dots and upconversion nanoparticles are presented. The results suggest that energy transfer from excited upconversion nanoparticles to quantum dots occurs upon self-assembly with short oligonucleotides. This example shows the potential of using DNA-based assembly as a general technique for creating novel materials helping to gain a fundamental understanding about nanoparticle interactions. In addition, lead halide perovskite nanoparticles are introduced. A modified synthesis protocol is demonstrated, which significantly increases the processability of such nanoparticles.
Supervisor: Kanaras, Antonios Sponsor: Not available
Qualification Name: Thesis (Ph.D.) Qualification Level: Doctoral
EThOS ID:  DOI: Not available