DNA-stabilized Silver Nanoclusters: From Photophysical Characterization to Bioimaging Applications

Publikation: Bog/antologi/afhandling/rapportPh.d.-afhandling

Abstract

DNA-stabilized silver nanoclusters (DNA-AgNCs) are fascinating emitters comprised of a few silver atoms that are stabilized by one or more DNA oligomers. Their emission tunability from the visible to near-infrared (NIR) range, high quantum yields, photostability, and biocompatibility make this class of emitters highly attractive. To promote DNA-AgNCs for applications, a fundamental understanding of their formation, structure, and properties is essential. My work in this research field included fundamental investigations of structural and spectroscopic properties as well as application-oriented studies.

Unraveling the correlation of the photophysical properties with the structure of the cluster is crucial for the prediction of DNA-AgNCs with tailored properties. However, only a few crystal structures are currently known, as obtaining high-quality crystals of DNA-AgNCs is challenging. My structure elucidation attempts resulted in a partially solved structure of a green-emitting DNA-AgNC.

Unfortunately, the encapsulating DNA structure remained unresolved, but the arrangement of the silver atoms in the cluster core was determined. Despite the missing information on the structural arrangement of the DNA, the cluster core already provides valuable insights into the structureproperty relationships.

Due to the advantages of the NIR transparency window, the discovery of DNA-AgNCs in this spectral region is of great interest. I have explored the fundamentals of a NIR-emitting DNA-AgNC with outstanding and unusual properties. The cluster shows a dual emissive behavior which can be used as a light intensity meter on the nanoscale.

DNA-AgNCs are promising candidates for biological applications. The success of their

implementation depends on the controlled and targeted conjugation. I investigated the rational conjugation using copper-free click chemistry. The key to ensure this rational conjugation strategy is a solved crystal structure. The NIR-emitting DNA-Ag16NC with a known structure was successfully linked to three different peptides and a small protein. The spectroscopic properties of the cluster remained unchanged and bioimaging studies demonstrated the large potential for biological applications.
OriginalsprogEngelsk
ForlagDepartment of Chemistry, Faculty of Science, University of Copenhagen
Antal sider212
StatusUdgivet - 2024

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