Rothenbühler, Simon (2022). DNA Architectonics: Self-Assembly of Amphiphilic Oligonucleotides into Supramolecular Nanostructures. (Thesis). Universität Bern, Bern
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22rothenbuehler_s.pdf - Thesis Available under License Creative Commons: Attribution-Noncommercial-No Derivative Works (CC-BY-NC-ND 4.0). Download (38MB) | Preview |
Abstract
The first chapter aims at introducing topics related to the thesis. These include supramolecular polymers in aqueous medium, some structural aspects of deoxyribonucleic acid (DNA), the preparation of synthetic oligomers, the concept of aggregation-induced emission (AIE), and different approaches for the construction of DNA nanostructures. This introduction, with a focus on what has been reported previously in our research group, is followed by elucidating the aim of the thesis in chapter 2. The results of the experimental lab work are discussed in the subsequent chapters. In the third chapter, amphiphilic DNA conjugates exhibiting hydrophobic tetraphenylethylene (TPE) sticky ends at the 3’-ends are examined. Supramolecular assembly of such DNA duplexes results in two distinct vesicular morphologies – they either appear as prolate ellipsoids or spheres. The two different DNA architectures are characterized by their DNA duplex alignment within the supramolecular arrays. Only one type of DNA packing leads to the formation of DNA-addressable vesicular constructs. The self-assembly of 3’-/5’-end TPE-modified DNA duplexes into vesicular nanostructures are explored in chapter 4. The objective of this chapter is to investigate the influence of the TPE sticky ends and DNA sequence length on the self-assembly behavior of the duplexes. The fifth chapter is devoted to further functionalize the supramolecular constructs, assembled from 3’-/5’-end TPE-modified DNA duplexes. Introduction of a terminal functionality into the duplexes governs the supramolecular assembly process and leads to clearly distinct DNA architectures, such as a star-shaped morphology. Chapter 6 provides an approach for the creation of DNA nanostructures, assembled from 3’-/5’-end TPE-modified DNA conjugates hybridized to a longer DNA complement. In the seventh chapter, the self-assembly of phosphodiester-linked TPE trimers in aqueous medium under different conditions is presented. Chapter 8 briefly describes a collaboration project, namely the synthesis of target compounds that are subsequently employed in on-surface polymerization and cryo-force spectroscopy experiments. Finally, overall conclusions are drawn, as well as outlining future perspectives.
| Item Type: | Thesis |
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| Dissertation Type: | Cumulative |
| Date of Defense: | 13 May 2022 |
| Subjects: | 500 Science > 540 Chemistry 500 Science > 570 Life sciences; biology 600 Technology > 610 Medicine & health |
| Institute / Center: | 08 Faculty of Science > Department of Chemistry, Biochemistry and Pharmaceutical Sciences (DCBP) |
| Depositing User: | Sarah Stalder |
| Date Deposited: | 06 Dec 2022 14:36 |
| Last Modified: | 13 May 2023 22:25 |
| URI: | https://boristheses.unibe.ch/id/eprint/3969 |
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