The 21st century marks the defining point of human history in terms of technological advancement. In 2014, we were at the edge of acquiring a complete understanding of the fundamental construct to all life forms. The capability to manipulate and recreate lives as desired will soon be at our hands and will eventually lead to the redefinition of life and humanity. This brave new world, for better or worse, will be stitched together by scientific breakthroughs in many disciplines. Nanopore fluidic system – and microfluidic in general – might be one of the key puzzles towards the future. It is seen as a likely candidate for the next generation of rapid and low-cost genetic sequencing technology, which will allow us to gain thorough insight into the genetic code of every living organism on earth. It can also have the capability to individually detect and manipulate virtually any biological molecules, possibly allowing it to be a universal diagnostic tool or a bio-molecule synthesiser. The future of nanopore fluidic system is prosperous, but the difficulties are equally challenging. Currently, both biological and solid-state nanopores are non-trivial to create. For instance, a small solid-state nanopore can only be fabricated with expansive machinery in a low-yield, low-throughput manner. To overcome this challenge, a new set of methods involving high electric field to fabricate and enlarge a solid-state nanopore has been developed. It was found that a nanopore, when subjected to a high electric field, can be enlarged in angstrom increments and cleared of unidentified obstructions that cause low-frequency ionic current fluctuations. It was also found that an intact solid-state membrane, when subjected to a high electric field for a period of time, can leave a single nanopore imprinted onto it. The process of creation is best describe as a dielectric breakdown event and can be modeled by the percolation theory for dielectric breakdown. The resulting nanopores are cylindrical in shape and are shown to be equally capable of single molecule sensing compare to pores created by other methods. To accommodate future nanopore designs and applications and to examine the scope of applicability of the new fabrication approach, more advanced nanopore devices were created on some dual-layer solid-state membranes comprising of a metallic and a dielectric layer. Experiments indicated that the method could indeed create nanopore on such advanced membranes. It was further shown that the metallic layer receded further than the dielectric layer, forming a hollow conical shape at the opening of the dielectric nanopore. Such metalized bi-layer nanopore system was found to interact strongly with short single stranded DNA molecules, resulting in prolonged DNA translocation time. A simple picture of the mechanism was proposed to explain the observation. Lastly, to extend the limit of the new fabrication approach, I attempted to fabricate nanopore on complex multi-layer membranes involving a graphene film sandwiched in several dielectric materials. It was found that the quality of the graphene film and the transfer method were vital to the success of this project. Nevertheless, preliminary results indicated that the new method could create a nanopore through this complex multi-layer membrane. The new method to fabricate and tune both simple and complex nanopores is amongst the simplest, the least costly and the most efficient one that one can imagine. The research work has already sparked a dramatic increase in scientific throughput in our laboratory and other laboratories we had collaboration with. It fueled more than a dozen projects and involved close to a thousand nanopores in total. Such projects are far from possible if they were to rely on conventional fabrication methods. However, these are insignificant if we consider the new method is simple enough that, for the very first time, general public can easily access nanofabrication and single-molecule manipulation technology. The liberation of nanotechnology to the general public symbolically marks the beginning of a brave new world.

Le micro-usinage de matériaux transparents est aujourd’hui un sujet d’intérêt mondial en recherche appliquée. L’emploi de lasers femtoseconde permet la micro-fabrication de composants optiques et de verres intelligents, ou la réalisation de cellules photovoltaïques. Dans ce contexte, cette thèse expérimentale se concentre sur l’absorption laser résolue en temps et en espace à la surface de matériaux diélectriques irradiés (silice fondue et saphir). Des impulsions femtoseconde (30 − 450 fs) dans l’infrarouge sont utilisées pour étudier l’efficacité de couplage de l’énergie laser pour l’ablation de matériaux dans un régime d’intensité intermédiaire (1-100 TW/cm²) lors de deux expériences. Un schéma pompe-sonde détermine la dynamique du plasma électrontrou à l’échelle femtoseconde et une expérience de déplétion laser mesure l’énergie absorbée. Une étude morphologique du matériau est réalisée, évaluant les seuils d’endommagement et d’ablation ainsi que les morphologies d’ablation. Nous établissons ensuite un bilan d’énergie de l’absorption laser responsable de l’enlèvement de matière. Les densités d’énergie typiques atteintes sont évaluées expérimentalement et confrontées à une modélisation avec propagation. Un excès de dépôt d’énergie par rapport à l’énergie de liaison du matériau au repos est mis en évidence, suggérant qu’un important chauffage du gaz d’électrons libres a lieu. Nous réalisons enfin une interprétation des données avec un regard technologique. Des guides à la réalisation de microsystèmes en régime d’ablation laser femtoseconde sont proposés, et démontrent l’intérêt d’impulsions sous 100 fs pour un procédé photonique. / This thesis concerns femtosecond laser absorption in dielectrics in the context of micromachining processes of glass materials. Prospected applications of this technology are optical component micro-fabrication, smart glass manufacturing, or photovoltaic cell patterning. In this context, we focus on the characterization in time and space of the absorption mechanisms occurring at the surface of irradiated dielectric materials (fused silica and sapphire). Using near-IR ultrashort pulses (30 − 450 fs) laser energy coupling efficiency for material ablation is studied at mid-intensities (1-100 TW/cm²) through two experiments. A pump-probe scheme determines the electron-hole plasma dynamics at femtosecond timescale and a laser depletion experiment measures the material absorption. A morphological study of the samples is performed, evaluating the damage and ablation thresholds as well as ablation morphologies. We then establish an energy balance of laser absorption responsible of matter removal. Typical energy densities reached are estimated through experiments and confronted to a propagative model. It is shown that the amount of absorbed energy is far above the bonding energy of the material at rest, suggesting that the major part of the absorbed energy is spent to heat the free electron gas. Finally, we propose a technological analysis of the experimental data. The interest of sub-100 fs laser pulses for photonic processes is evidenced, however at the cost of additional complexity. It provides guidelines for efficient direct laser ablation, making the results relevant for femtosecond processes.

Initial research in the field of organic electronics focused primarily on the improvements in material performance. Significant progress has been achieved in the case of organic field effect transistors, where reported mobility values are now over 5 orders of magnitude higher than those of early devices. As a consequence, the use of organic transistors is now being considered for real-world applications in the form of integrated logic circuits. This in turn presents many new challenges, as the logic circuit requirements are more demanding on the transistor characteristics and corresponding fabrication processes. This thesis investigates the feasibility of organic technology for its potential use in future low-cost, high-volume electronic applications. The research objectives were accomplished by practical evaluation of an organic logic circuit fabrication process. First, recent advances in the fabrication of organic circuits in terms of transistor structure, material usage and fabrication techniques are reviewed. Next, a lithographic logic circuit fabrication process using PVP gate dielectric and TIPS-pentacene organic semiconductor adapted from state of the art fabrication process is presented. The logic circuit design decisions and the methodology for the fabrication process are thoroughly documented. Using this process, zero-Vgs and diode-load inverter circuits were successfully fabricated. However, the process is in need of further refinement for more complex circuit designs, as the fabrication of a comparator circuit consisting of 11 transistors was unsuccessful. Two optimisation techniques that are compatible with the logic circuit fabrication process were also explored in this work. To improve the capacitive coupling of the dielectric layer, the use of a polymer nanocomposite dielectric was investigated. The nanocomposite is prepared by blending PVP solution with a high-k inorganic nanoparticle filler, barium strontium titanate. Using the nanocomposite dielectric, both single transistors and integrated logic circuits were successfully fabricated. This is the first report on the use of PVP and barium strontium titanate nanocomposite dielectric with a lithographic based logic circuit fabrication process. The use of PFBT modified Au contacts for the fabrication process was investigated to improve theperformance of the contact electrode layer. Using PFBT, mobility increased by one order of magnitude over untreated Au electrodes for the PVP and TIPS-pentacene transistors.

The first microwave measurement techniques uses an open ended coaxial probe with a purposely built sample holder to measure the dielectric properties of potato products from 500 MHz to 1 GHz. The second system utilises a waveguide cell with a purposely built sample holder to characterise potato products from 2.4 to 3.5 GHz. Common British varieties of raw potatoes such as Estima, King Edward and Maris Piper are used in this study. The two microwave measurement techniques are also used to measure the dielectric properties of potato products at elevated temperatures for these frequency ranges. Both measurement techniques are also used to study the effect of storage temperature on the dielectric properties of Saturna raw potato. For this part of the study, it is concluded that the microwave measurement techniques are unable to discriminate between potatoes that had a storage history of different temperature profiles. On the other hand, waveguide cells and open ended coaxial probes are able to measure the dielectric properties of raw potato, partial cooked fried potato and fried potato at the 500 MHz to 1 GHz and 2.4 GHz to 3.5 GHz frequency range. The measurement results show that both dielectric constant and loss values of fried potatoes decreased with frying time, due to the reduced moisture content during the frying process. Furthermore, the dielectric loss behaviour of raw and fried potatoes is dominated by the effect of the ionic conductivity at frequencies lower than 1 GHz. An apparatus has been designed and built in order to measure the dielectric properties of potato for both frequency ranges as a function of temperature. In the subsequent measurements it is found that the dielectric properties of potato products at elevated temperatures also depend on frequency and moisture content. For high moisture content potato (~> 70 %), at 2.45 GHz both the dielectric constant and loss are found to decrease with temperature, whereas at 915 MHz the dielectric constant decreases but the loss increases for the moisture content above 30%. For the intermediate moisture content (10%<MC<70%), all dielectric properties increase with temperature at the microwave heating frequencies 2.45GHz, whereas at 915 MHz all the dielectric properties increase with temperature for the moisture content range 10% to 30%. The increase in dielectric properties with temperature is small and marginal for fried potatoes with low moisture content (< 10 %). It is therefore apparent that moisture content is the primary factor in detecting the complex permittivity of potato products.

The aim of this thesis is to identify coupling mechanisms for three line microstrip, stripline and microstrip with dielectric overlay structures as either inductive or capacitive, quantify through simulation and measurement the amount of crosstalk to be expected in terms of scattering parameters. A new method of crosstalk suppression is implemented into each three line structure by placing uniformly spaced short circuits down the length of the center transmission line. All structures were simulated over various physical and electrical parameters. Select microstrip structures, shielded and unshielded, were fabricated and measured to validate the effectiveness of the shielding technique. Shielding effectiveness was calculated from the measurements, and their results showed that the isolation between lines was increased by up to 20dB.

Neste trabalho foi investigado o processo de relaxação em copolímeros metacrilicos funcionalizados com o grupo cromóforo 4-[N-etil-N-(2-hidroxietil)]amino-2\'-cloro-4\'nitro-azobenzeno (MMADRI3). Os copolímeros sintetizados foram caracterizados por espectrofotometria de visível e infravermelho, calorimetria diferencial de varredura, análise termogravimétrica e elipsometria. O triodo de corona foi utilizado para induzir a orientação dos cromóforos dipolares a temperaturas próximas da transição vítrea. Os valores do coeficiente eletroóptico linear r13 de filmes obtidos por derramento de solução podem alcançar 14 pm/V em amostras funcionalizadas com 43%de cromóforo.O efeito piezoelétricoé significativo para amostras contendo 4% de cromóforo sendo a sua origem atribuída à carga espacial. A relaxação orientacional dos cromóforos foi estudada medindo-se o decaimento do coeficiente eletroóptico e a relaxação dielétrica a diferentes temperaturas. O processo de relaxação foi interpretado utilizando a equação de Kohlraush-Williams-Watts (KWW) aplicada aos domínios do tempo e da freqüência. O tempo de relaxação característico &#964 e o parâmetro b da equação de KWW foram obtidos como função da temperatura desde a temperatura ambiente até acima da temperatura de transição vítrea. O parâmetro b à temperatura de transição vítrea aproxima-se de 0,6 valor que é atribuído a forças de curto alcance. As medidas dielétricas revelaram duas bandas de relaxação &#946 e &#945 respectivamente a baixas e a altas temperaturas. A relaxação a está relacionada com a transição vítrea e à desorientação dos cromóforos. A dependência de &#964 foi fundamentada nas equações de Arrhenius e de Vogel-Fulcher-Tarmnann-Hesse (VFTH), respectivamente a baixas e a altas temperaturas. Os parâmetros de VFTH encontram-se próximos dos considerados universais. O comportamento de &#964 em toda a gama de temperaturas, foi explicado pela equação de Adam-Gibbs, usando-se os parâmetros de VFTH. O resfriamento a taxas lentas após o processo de polarização aumenta substancialmente o tempo de relaxação e a sua energia de ativação. Os expoentes m e n do modelo de Dissado-Hill baseado na interação de multicorpos foram obtidos em função da temperatura. Os valores do parâmetro n ficam dentro do esperado pela teoria / The relaxation process of side-chain methacrylate copolymers functionalized with the nonlinear optical azo chromophore 4-[Nethyl-N-(2-hydroxyethyl)]-amino-2\'-chloro-4-nitroazobenzene (MMADR13) was investigated. The copolymers synthesized were characterized by visible and infrared spectrophotometry, differential scanning calorimetry, thermogravimetric analysis and ellipsometry. The corona triode was employed to induce the orientation of the dipolar chromophore at a temperature near the glass transition. The linear eletrooptic coefficient r13 of cast fllms can reach values as high as 14 pm/V in samples with 43% of chromophore contento The piezoeletric effect attributed to space charge was only significant in the lowest chromophore content samples (4%). Electrostriction was shown to affect to some extent the quadratic electrooptic measurements. The chromophore relaxation at different temperatures was investigated by both electrooptic decay and dielectric measurements. The relaxation process was interpreted using the Kohlraush-Williams-Watts (KWW) equation both in the time and frequency domains. From the KWW equation the characteristic relaxation time &#964 and the stretching parameter b were obtained from room temperature to temperatures above the glass transition. Near the glass transition b is ca 0.6 which is characteristic of short range interactions. Dielectric measurements revealed two relaxation bands, &#946 and &#945, at low and high temperatures, respectively. The &#945 relaxation was attributed to the glass transition and to the 10ss of chromophore orientational order. The temperature behavior of &#964 was interpreted by the Arrhenius and Vogel-Fulcher-Tammann-Hesse (VFTH) equations. at low and high temperatures. respectivelly. The VFTH parameters lie close to the so-called universal values. In addition the overall temperature dependence was explained by the Adam-Gibbs equation using the VFTH parameters. Using a small cooling rate after corona poling increases substantially the relaxation time and the activation energy .The power law exponents m and n. from Dissado-Hill manybody interactions model were obtained as a function of temperature. The n values are in the range of expected values for the many-body interactions model

abstract: The chemical, structural, and electrical properties of niobium-silicon, niobium-germanium, and YBCO-dielectric interfaces are characterized. Reduction in the concentration of interfacial defects in these structures can improve the performance of (i) many devices including low-loss coplanar, microstrip, and stripline microwave resonators used in next-generation cryogenic communication, sensor, and quantum information technologies and (ii) layers used in device isolation, inter-wiring dielectrics, and passivation in microwave and Josephson junction circuit fabrication. Methods were developed to synthesize amorphous-Ge (a-Ge) and homoepitaxial-Si dielectric thin-films with loss tangents of 1–2×10 -6 and 0.6–2×10 -5 at near single-photon powers and sub-Kelvin temperatures (≈40 mK), making them potentially a better choice over undoped silicon and sapphire substrates used in quantum devices. The Nb/Ge interface has 20 nm of chemical intermixing, which is reduced by a factor of four using 10 nm Ta diffusion layers. Niobium coplanar resonators using this structure exhibit reduced microwave losses. The nature and concentration of defects near Nb-Si interfaces prepared with commonly-used Si surface treatments were characterized. All samples have H, C, O, F, and Cl in the Si within 50 nm of the interface, and electrically active defects with activation energies of 0.147, 0.194, 0.247, 0.339, and 0.556 eV above the valence band maximum (E vbm ), with concentrations dominated by a hole trap at E vbm +0.556 eV (presumably Nb Si ). The optimum surface treatment is an HF etch followed by an in-situ 100 eV Ar ion mill. RCA etches, and higher energy ion milling processes increase the concentration of electrically active defects. A thin SrTiO 3 buffer layer used in YBa 2 Cu 3 O 7-δ superconductor/high-performance Ba(Zn 1/3 Ta 2/3 )O 3 and Ba(Cd 1/3 Ta 2/3 )O 3 microwave dielectric trilayers improves the structural quality of the layers and results in 90 K superconductor critical temperatures. This advance enables the production of more compact high-temperature superconductor capacitors, inductors, and microwave microstrip and stripline devices. / Dissertation/Thesis / Doctoral Dissertation Materials Science and Engineering 2020

Hafnium based high-κ dielectrics are considered potential candidates to replace SiO2 or SiON as the gate dielectric in complementary metal oxide semiconductor (CMOS) devices. Hydrogen is one of the most significant elements in semiconductor technology because of its pervasiveness in various deposition and optimization processes of electronic structures. Therefore, it is important to understand the properties and behavior of hydrogen in semiconductors with the final aim of controlling and using hydrogen to improve electronic performance of electronic structures. Trap transformations under annealing treatments in hydrogen ambient normally involve passivation of traps at thermal SiO2/Si interfaces by hydrogen. High-κ dielectric films are believed to exhibit significantly higher charge trapping affinity than SiO2. In this thesis, study of hydrogen trapping in alternate gate dielectric candidates such as HfO2 during annealing in hydrogen ambient is presented. Rutherford backscattering spectroscopy (RBS), elastic recoil detection analysis (ERDA) and nuclear reaction analysis (NRA) were used to characterize these thin dielectric materials. It was demonstrated that hydrogen trapping in bulk HfO2 is significantly reduced for pre-oxidized HfO2 prior to forming gas anneals. This strong dependence on oxygen pre-processing is believed to be due to oxygen vacancies/deficiencies and hydrogen-carbon impurity complexes that originate from organic precursors used in chemical vapor depositions (CVD) of these dielectrics.

No description available.

京都大学 / 0048 / 新制・課程博士 / 博士(工学) / 甲第22159号 / 工博第4663号 / 新制||工||1727(附属図書館) / 京都大学大学院工学研究科材料工学専攻 / (主査)教授 田中 功, 教授 中村 裕之, 教授 邑瀬 邦明 / 学位規則第4条第1項該当 / Doctor of Philosophy (Engineering) / Kyoto University / DFAM