Kyoto University (京都大学) / 0048 / 新制・課程博士 / 博士(工学) / 甲第16866号 / 工博第3587号 / 新制||工||1542(附属図書館) / 29541 / 京都大学大学院工学研究科材料化学専攻 / (主査)教授 平尾 一之, 教授 田中 勝久, 教授 三浦 清貴 / 学位規則第4条第1項該当

This thesis report works on optically characterizing waveguide based biosensors consisting of thin, narrow Au stripes embedded in CYTOP. The devices were examined using an ever evolving and improving interrogation setup, variations of which are described in detail in this document. A number of changes were made to the setup configuration in order to reduce noise levels and increase efficiency and accuracy of acquired measurements. Waveguides of varying configurations (straight waveguides and Mach-Zehnder Interferometers with etched and cladded channels) are described and optically characterized. The characterization results of these devices are presented in this thesis. Bulk index measurements are carried out in order to determine a suitable bio-sensing solution with a refractive index matched to that of CYTOP. Step index measurements clearly distinguishing the introduction of sensing solutions of refractive indices varying from one another, are made available. Preliminary bio-sensing experiments involving detection of change in refractive index of sensing fluid as well as adlayer thickness with the introduction of analytes binding to the waveguide surface that has been functionalized with antibodies, using both straight and cladded waveguides with single mode outputs are studied.

This thesis details the fabrication of three different plasmon-polariton based devices: a plasmon-polariton Bragg grating (PPBG) biosensor, an intensity modulator incorporating grating couplers, and optically separated electrical contact, and finally an array of nanoholes in an ultrasmooth Au film. The biosensor involves a 35 nm Au stripe, lithographically stepped in width to produce a Bragg reflector. The waveguide is embedded in symmetric, Cytop claddings 8 µm thick. Channels are etched into the top cladding, exposing the waveguides and allowing for the integration of fluidics. The modulator involves a 20 nm Au pad, overlaid with 80 nm Au diffraction gratings, supported by an ultrathin (~3 nm) SiO2 insulator, on a p-doped Silicon wafer backed by an Al Ohmic contact. Electrical contact pads are separated from the waveguide by a thick dielectric (700 nm PMMA), and 2.5 µm vias in-filled with Au allow for electrical connection between the contact pads and waveguides. The nanohole array is machined by focused ion beam into an ultrasmooth Au film revealed by template stripping. The Au film is stacked on a thick film of Cytop between ~5 µm thick.

Group- III nitride based semiconductors have emerged as the leading material for short wavelength optoelectronic devices. The InGaN alloy system forms a continuous and direct bandgap semiconductor spanning ultraviolet (UV) to blue/green wavelengths. An ideal and highly efficient light-emitting device can be designed by enhancing the spontaneous emission rate. This thesis deals with the design and fabrication of a visible light-emitting device using GaN/InGaN single quantum well (SQW) system with enhanced spontaneous emission. To increase the emission efficiency, layers of different metals, usually noble metals like silver, gold and aluminum are deposited on GaN/InGaN SQWs using metal evaporator. Surface characterization of metal-coated GaN/InGaN SQW samples was carried out using atomic force microscopy (AFM) and scanning electron microscopy (SEM). Photoluminescence is used as a tool for optical characterization to study the enhancement in the light emitting structures. This thesis also compares characteristics of different metals on GaN/InGaN SQW system thus allowing selection of the most appropriate material for a particular application. It was found out that photons from the light emitter couple more to the surface plasmons if the bandgap of former is close to the surface plasmon resonant energy of particular metal. Absorption of light due to gold reduces the effective mean path of light emitted from the light emitter and hence quenches the quantum well emission peak compared to the uncoated sample.

Surface Plasmon Resonance (SPR) and localized surface plasmon resonance (LSPR) biosensors have brought a revolutionary change to in vitro study of biological and biochemical processes due to its ability to measure extremely small changes in surface refractive index (RI), binding equilibrium and kinetics. Strategies based on LSPR have been employed to enhance the sensitivity for a variety of applications, such as diagnosis of diseases, environmental analysis, food safety, and chemical threat detection. In LSPR spectroscopy, absorption and scattering of light are greatly enhanced at frequencies that excite the LSPR, resulting in a characteristic extinction spectrum that depends on the RI of the surrounding medium. Compositional and conformational change within the surrounding medium near the sensing surface could therefore be detected as shifts in the extinction spectrum. This dissertation specifically focuses on the development and evaluation of highly sensitive LSPR biosensors for in situ study of biomolecular binding process by incorporating nanotechnology. Compared to traditional methods for biomolecular binding studies, LSPR-based biosensors offer real-time, label free detection. First, we modified the gold sensing surface of LSPR-based biosensors using nanomaterials such as gold nanoparticles (AuNPs) and polymer to enhance surface absorption and sensitivity. The performance of this type of biosensors was evaluated on the application of small heavy metal molecule binding affinity study. This biosensor exhibited ~7 fold sensitivity enhancement and binding kinetics measurement capability comparing to traditional biosensors. Second, a miniaturized cell culture system was integrated into the LSPR-based biosensor system for the purpose of real-time biomarker signaling pathway studies and drug efficacy studies with living cells. To the best of our knowledge, this is the first LSPR-based sensing platform with the capability of living cell studies. We demonstrated the living cell measurement ability by studying the VEGF signaling pathway in living SKOV-3 cells. Results have shown that the VEGF secretion level from SKOV-3 cells is 0.0137 ± 0.0012 pg per cell. Moreover, we have demonstrated bevacizumab drug regulation to the VEGF signaling pathway using this biosensor. This sensing platform could potentially help studying biomolecular binding kinetics which elucidates the underlying mechanisms of biotransportation and drug delivery.

This project was focused on the creation of a gold-coated grating structure capable of inducing a surface plasmon polariton within the mid-infrared region, enhancing emissions at specific wavelengths based on the grating periodicity. The grating structure was formed on a silicone elastomer, polydimethylsiloxane (PDMS), in order to give the structure, the ability to have the periodicity dimensions of the grating altered by applying a stress, thereby changing the location of the emission enhancement, giving the device the potential to be used as an infrared strain sensor. Creation of the structure employed a top-down, micro-scale fabrication technique referred to as Direct Laser Writing (DLW). Using a light-sensitive, negative-tone photoresist material, a grating was patterned onto a glass substrate via photopolymerization, in which areas exposed to an ultraviolet (UV) laser were rendered insoluble by forming cross-links on the portions of the resist which interacted with the UV source. This grating was then placed under a custom-designed mold which was then filled with liquid PDMS and cured for 3 hours at 60°C to cure (harden or cross-link) and leaving an inverse elastomer pattern behind once the cured PDMS was peeled off the substrate. Upon coating the structure with a ~80 nm thick layer of gold, a Fourier Transform infrared (FTIR) spectrometer was used to measure the thermal emissions spectrum of the sample grating at a high temperature (~200°C) and under different strains. These spectra were then analyzed to look for selective emission enhancements caused by the grating structure due to the inducing of a surface plasmon polariton (SPP), as well as changes in the location and nature of these enhancements based on applied strains. Final results showed two sets of enhancement behaviors with the application of uniaxial strain: a shifting of the region of peak emission enhancement to higher wavelengths, and a broadening of the region of enhancement. However, more testing is needed in order to determine the precise causes of the behavior and to quantify it in such a way that it could be turned into a functioning sensor device.

This master’s thesis deals with the plasmon resonance of the nanostructures of several selected tungsten oxides using Fourier transform infrared spectroscopy (FTIR spectroscopy). The physical principles of the plasmonics, the characteristics of the materials used, as well as the principle of operating and measuring on the FTIR spectrometer, are described in the first part of this thesis. The second part is focused on the preparation of samples and performing measurements on the FTIR spectrometer. This part ends by representing the final spectra and the results obtained.

No description available.

Glucans are cell wall constituents of fungi and bacteria that bind to pattern recognition receptors and modulate innate immunity, in part, by macrophage activation. We used surface plasmon resonance to examine the binding of glucans, differing in fine structure and charge density, to scavenger receptors on membranes isolated from human monocyte U937 cells. Experiments were performed at 25°C using a biosensor surface with immobilized acetylated low density lipoprotein (AcLDL). Inhibition of the binding by polyinosinic acid, but not polycytidylic acid, confirmed the interaction of scavenger receptors. Competition studies showed that there are at least two AcLDL binding sites on human U937 cells. Glucan phosphate interacts with all sites, and the CM-glucans and laminarin interact with a subset of sites. Polymer charge has a dramatic effect on the affinity of glucans with macrophage scavenger receptors. However, it is also clear that human monocyte scavenger receptors recognize the basic glucan structure independent of charge.

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第18979号 / 工博第4021号 / 新制||工||1619(附属図書館) / 31930 / 京都大学大学院工学研究科マイクロエンジニアリング専攻 / (主査)教授 鈴木 基史, 教授 木村 健二, 教授 蓮尾 昌裕 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM