Synthesis and characterization of DNA-single molecule-DNA triblock structures : as a novel approach towards single-molecule electronics

Placeholder Show Content

Abstract/Contents

Abstract
A precise and reproducible electrical contact between a single molecule and the electrodes is the first step in studying single-molecule electronics, which uses individual molecules as active electronic components. One potentially promising strategy to make the electrical contact to a single molecule is to use DNA as a template. DNA has emerged as a good scaffold in the field of nanoelectronics because DNA is easily aligned over large areas, and can be employed as a conducting nanowire with micrometer-scaled length after metallization using metal ions. Moreover, oligodeoxynucleotide (ODN) can be readily linked to a single organic molecule, and its length can be further increased to several micrometer scales through DNA extension techniques. To build DNA-assist single-molecule device structures, I investigated the reactivity of ODN to synthesize organic molecule-bis(ODN) triblock oligomers through three separate cross-coupling routes, such as amide-coupling reaction, isothiourea-bond formation, and "click" chemistry. Specifically, the amide-coupling reaction is scrutinized to enhance its reactivity since it affords the highest yield among the cross-coupling reactions. The optimized amide-coupling reaction is also employed to incorporate functional organic molecules, involving a fluorophore and a conjugated polymer, into ODNs. Organic molecule-bis(ODN) triblock oligomers were characterized by denaturing gel electrophoresis and electrospray ionization mass spectrometry. The ODNs of the triblock oligomers are elongated by polymerase chain reaction (PCR) or DNA hybridization/ligation methods. PCR is a fast and precise method to construct organic molecule-bis(1.5 kbp dsDNA) triblock structures from the triblock oligomers. On the other hand, DNA hybridization/ligation affords longer length of the ODN using micrometer-sized DNA fragments, which are prepared from lambda DNA using restriction enzymes and a phosphatase. Thus, organic molecule-bis(micrometer-sized DNA) triblock structures are assembled to obtain fully stretched DNA strands. To characterize the triblock structures, fluorophore-bis(micrometer-sized DNA) triblock structure was synthesized through DNA hybridization/ligation, and then directly imaged by combined atomic force and single-molecule fluorescence microscopy. For the purpose of building a single-molecule transistor device, a conjugated polymer-bis(micrometer-sized DNA) triblock structure was metallized by palladium metal ion. The metallized triblock structure is characterized by scanning electron microscopy (SEM) to monitor a nanogap from the conjugated polymer (contour length: ~7 nm). Unfortunately, the nanogap is not observed, due to overgrowth of metal ions during the DNA metallization. To overcome the problem, I also describe the synthesis of a micrometer-sized DNA-conjugated polymer-gold nanoparticle asymmetric triblock structure.

Description

Type of resource text
Form electronic; electronic resource; remote
Extent 1 online resource.
Publication date 2010
Issuance monographic
Language English

Creators/Contributors

Associated with Lee, Jung Kyu
Associated with Stanford University, Department of Chemistry
Primary advisor Bao, Zhenan
Thesis advisor Bao, Zhenan
Thesis advisor Chidsey, Christopher E. D. (Christopher Elisha Dunn)
Thesis advisor Waymouth, Robert M
Advisor Chidsey, Christopher E. D. (Christopher Elisha Dunn)
Advisor Waymouth, Robert M

Subjects

Genre Theses

Bibliographic information

Statement of responsibility Jung Kyu Lee.
Note Submitted to the Department of Chemistry.
Thesis Thesis (Ph.D.)--Stanford University, 2010.
Location electronic resource

Access conditions

Copyright
© 2010 by Jung Kyu Lee
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

Also listed in

Loading usage metrics...