京都大学 / 0048 / 新制・課程博士 / 博士(理学) / 甲第19525号 / 理博第4185号 / 新制||理||1601(附属図書館) / 32561 / 京都大学大学院理学研究科化学専攻 / (主査)教授 杉山 弘, 教授 三木 邦夫, 教授 藤井 紀子 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

No description available.

Bottom-up self-assembly can be used to create structures with sub-20 nm feature sizes or materials with advanced electrical properties. Here I demonstrate processes to enable such self-assembling systems including block copolymers and DNA origami, to be integrated into nanoelectronic devices. Additionally, I present a method which utilizes the high stability and electrical conductivity of graphene, which is a material formed using a bottom-up growth process, to create archival data storage devices. Specifically, I show a technique using block copolymer micelle lithography to fabricate arrays of 5 nm gold nanoparticles, which are chemically modified with a single-stranded DNA molecule and used to chemically attach DNA origami to a surface. Next, I demonstrate a method using electron beam lithography to control location of nanoparticles templated by block copolymer micelles, which can be used to enable precise position of DNA origami on a surface. To allow fabrication of conductive structures from a DNA origami template, I show a method using site-specific attachment of gold nanoparticles to and a subsequent metallization step to form continuous nanowires. Next, I demonstrate a long-term data storage method using nanoscale graphene fuses. Top-down electron beam lithography was used to pattern atomically thin sheets of graphene into nanofuses. To program the fuses, graphene is oxidized as the temperature of the fuse is raised via joule heating under a sufficiently high applied voltage. Finally, I investigate the effect of the fuse geometry and the electrical and thermal properties of the fuse material on the programming requirements of nanoscale fuses. Programming voltages and expected fuse temperatures obtained from finite element analysis simulations and a simple analytical model were compared with fuses fabricated from tellurium, a tellurium alloy, and tungsten.

No description available.

DNA origami templates have been studied due the versatility of shapes that can be designed and their compatibility with various materials. This has potential for future electronic applications. This work presents studies performed on the electrical properties of DNA origami templated gold nanowires. Using a DNA origami tile, gold nanowires are site specifically attached in a “C” shape, and with the use of electron beam induced deposition of metal, electrically characterized. These wires are electrically conductive with resistivities as low as 4.24 x 10-5 Ω-m. During moderate temperature processing nanowires formed on DNA origami templates are shown to be affected by the high surface mobility of metal atoms. Annealing studies of DNA origami gold nanowires are conducted, evaluating the effects of atom surface mobility at various temperatures. It is shown that the nanowires separate into individual islands at temperatures as low as 180° C. This work shows that with the use of a polymer template the temperature at which island formation occurs can be raised to 210° C. This could allow for post processing techniques that would otherwise not be possible.

No description available.

No description available.

京都大学 / 新制・課程博士 / 博士(理学) / 甲第23724号 / 理博第4814号 / 新制||理||1689(附属図書館) / 京都大学大学院理学研究科化学専攻 / (主査)教授 杉山 弘, 教授 深井 周也, 教授 秋山 芳展 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

This thesis forms part of an ongoing project in the DNA Group to build and operate a synthetic ribosome. We present two synthetic ribosome designs that can be combined with DNA-templated chemistry to generate libraries of functional synthetic small molecules. In Chapter 2 we use the DNA strand displacement technique to construct a mechanism that is capable of moving along a DNA track. We explore ways to control the speed and the driving force of the mechanism, and present a mathematical model of the system. We discuss the ability of the design to incorporate chemically-functionalised DNA strands. In Chapter 3 we use a 2D DNA origami tile as the basis of the synthetic ribosome mechanism. Functionalised DNA strands are arranged on the surface of the tile, and we demonstrate the ability to template reactions between the strands, and discuss the possibility of creating a library of distinct chemical products from a single origami tile.

In the past decade, DNA origami self-assembly has been widely applied for creating customised nanostructures with base-pair precision. In this technique, the unique chemical addressability of DNA can be harnessed to create programmable architectures, using components ranging from dye or protein molecules to metallic nanoparticles. In this thesis, we apply DNA nanotechnology for developing novel light-harvesting and optical voltage sensing nano-devices. We use the programmable positioning of dye molecules on a DNA origami plate as a mimic of a light-harvesting antenna complex required for photosynthesis. Such a structure allows us to systematically analyse optimal design concepts using different dye arrangements. Complementary to this, we use the resistive-pulse sensing technique in a range of electrolytes to characterise the mechanical responses of DNA origami structures to the electric field applied. Based on this knowledge, we assemble voltage responsive DNA origami structures labelled with a FRET pair. These undergo controlled structural changes upon application of an electric field that can be detected through a change in FRET efficiency. Such a DNA-based device could ultimately be used as a sensitive voltage sensor for live-cell imaging of transmembrane potentials.