京都大学 / 新制・課程博士 / 博士(理学) / 甲第23457号 / 理博第4751号 / 新制||理||1681(附属図書館) / 京都大学大学院理学研究科化学専攻 / (主査)准教授 前里 光彦, 教授 北川 宏, 教授 竹腰 清乃理 / 学位規則第4条第1項該当 / Doctor of Science / Kyoto University / DGAM

Title: Nutritional supplements as permitted doping Objectives: The main goal of this thesis is to find out for what specific reasons users of additional resources are willing to invest their money in the purchase of supplements, and also what is the decisive factor in choosing a particular type of product. Methods: To find out the knowledge of people sports at a professional or amateur level in the field of nutritional supplements, the method of questionnaire sociological survey was used. This method was used in order to determine the awareness of athletes about this topic, their possible influence by advertising or product prices, and also to ensure the complete anonymity of respondents. Results: This thesis describes the topic of nutritional supplements among athletes across all possible sports. We have found that the sports population has a very good overview of nutritional supplements, but at the same time it does not give as much of the right balance of their food. Keywords: sport, management, marketing, nutritional supplements, doping, prohibited substances

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Silicon carbide is a promising semiconductor material for high voltage, high frequency and high temperature devices due to its wide bandgap, high breakdown electric field strength, highly saturated drift velocity of electrons and outstanding thermal conductivity. With the aim of overcoming some challenges in metallization and doping during the fabrication of silicon carbide devices, a novel laser-based process is provided to direct metallize the surface of silicon carbide without metal deposition and dope in silicon carbide without high temperature annealing, as an alternative to the conventional ion implantation, and find applications of this laser direct write metallization and doping technique on the fabrication of diodes, endotaxial layer and embedded optical structures on silicon carbide wafers. Mathematical models have been presented for the temperature distributions in the wafer during laser irradiation to optimize laser process parameters and understand the doping and metallization mechanisms in laser irradiation process. Laser irradiation of silicon carbide in a dopant-containing ambient allows to simultaneously heating the silicon carbide surface without melting and incorporating dopant atoms into the silicon carbide lattice. The process that dopant atoms diffuse into the bulk silicon carbide by laser-induced solid phase diffusion (LISPD) can be explained by considering the laser enhanced substitutional and interstitial diffusion mechanisms. Nitrogen and Trimethyaluminum (TMA) are used as dopants to produce n-type and p-type doped silicon carbide, respectively. Two laser doping methods, i.e., internal heating doping and surface heating doping are presented in this dissertation. Deep (800 nm doped junction for internal heating doping) and shallow (200 nm and 450 nm doped junction for surface heating doping) can be fabricated by different doping methods. Two distinct diffusion regions, near-surface and far-surface regions, were identified in the dopant concentration profiles, indicating different diffusion mechanisms in these two regions. The effective diffusion coefficients of nitrogen and aluminum were determined for both regions by fitting the diffusion equation to the measured concentration profiles. The calculated diffusivities are at least 6 orders of magnitude higher than the typical values for nitrogen and aluminum, which indicate that laser doping process enhances the diffusion of dopants in silicon carbide significantly. No amorphization was observed in laser-doped samples eliminating the need for high temperature annealing. Laser direct metallization can be realized on the surface of silicon carbide by generating metal-like conductive phases due to the decomposition of silicon carbide. The ohmic property of the laser direct metallized electrodes can be dramatically improved by fabricating such electrodes on laser heavily doped SiC substrate. This laser-induced solid phase diffusion technique has been utilized to fabricate endolayers in n-type 6H-SiC substrates by carbon incorporation. X-ray energy dispersive spectroscopic analysis shows that the thickness of endolayer is about 100 nm. High resolution transmission electron microscopic images indicate that the laser endotaxy process maintains the crystalline integrity of the substrate without any amorphization. Rutherford backscattering studies also show no amorphization and evident lattice disorder occur during this laser solid phase diffusion process. The resistivity of the endolayer formed in a 1.55 omega•cm silicon carbide wafer segment was found to be 1.1E5 omega•cm which is sufficient for device fabrication and isolation. Annealing at 1000 oC for 10 min to remove hydrogen resulted in a resistivity of 9.4E4 omega•cm. Prototype silicon carbide PIN diodes have been fabricated by doping the endolayer and parent silicon carbide epilayer with aluminum using this laser-induced solid phase diffusion technique to create p-regions on the top surfaces of the substrates. Laser direct metallized contacts were also fabricated on selected PIN diodes to show the effectiveness of these contacts. The results show that the PIN diode fabricated on a 30 nm thick endolayer can block 18 V, and the breakdown voltages and the forward voltages drop at 100 A/cm2 of the diodes fabricated on 4H-SiC with homoepilayer are 420 ~ 500 V and 12.5 ~ 20 V, respectively. The laser direct metallization and doping technique can also be used to synthesize embedded optical structures, which can increase 40% reflectivity compared to the parent wafer, showing potential for the creation of optical, electro-optical, opto-electrical, sensor devices and other integrated structures that are stable in high temperature, high-pressure, corrosive environments and deep space applications.

Cerium oxide has been used extensively for various applications over the past two decades. The use of cerium oxide nanoparticles is beneficial in present applications and can open avenues for future applications. The present study utilizes the microemulsion technique to synthesize uniformly distributed cerium oxide nanoparticles. The same technique was also used to synthesize cerium oxide nanoparticles doped with trivalent elements (La and Nd). The fundamental study of cerium oxide nanoparticles identified variations in properties as a function of particle size and also due to doping with trivalent elements (La and Nd). It was found that the lattice parameter of cerium oxide nanoparticles increases with decrease in particle size. Also Raman allowed mode shift to lower energies and the peak at 464 cm-1 becomes broader and asymmetric. The size dependent changes in cerium oxide were correlated to increase in oxygen vacancy concentration in the cerium oxide lattice. The doping of cerium oxide nanoparticles with trivalent elements introduces more oxygen vacancies and expands the cerium oxide lattice further (in addition to the lattice expansion due to the size effect). The lattice expansion is greater for La-doped cerium oxide nanoparticles compared to Nd-doping due to the larger ionic radius of La compared to Nd, the lattice expansion is directly proportional to the dopant concentration. The synthesized cerium oxide nanoparticles were used to develop an electrochemical biosensor of hydrogen peroxide (H2O2). The sensor was useful to detect H2O2 concentrations as low as 1µM in water. Also the preliminary testing of the sensor on tomato stem and leaf extracts indicated that the sensor can be used in practical applications such as plant physiological studies etc. The nanomolar concentrations of cerium oxide nanoparticles were also found to be useful in decreasing ROS (reactive oxygen species) mediated cellular damages in various in vitro cell cultures. Cerium oxide nanoparticles reduced the cellular damages to the normal breast epithelial cell line (CRL 8798) induced by X-rays and to the Keratinocyte cell line induced by UV irradiation. Cerium oxide nanoparticles were also found to be neuroprotective to adult rat spinal cord and retinal neurons. We propose that cerium oxide nanoparticles act as free radical scavenger (via redox reactions on its surface) to decrease the ROS induced cellular damages. Additionally, UV-visible spectroscopic studies indicated that cerium oxide nanoparticles possess auto-regenerative property by switching its oxidation state between Ce3+ and Ce4+. The auto-regenerative antioxidant property of these nanoparticles appears to be a key component in all the biological applications discussed in the present study.

This work establishes a solid foundation for the use of indirect band gap semiconductors for light emitting application and presents the work on development of white light emitting diodes (LEDs) in silicon carbide (SiC). Novel laser doping has been utilized to fabricate white light emitting diodes in 6H-SiC (n-type N) and 4H-SiC (p-type Al) wafers. The emission of different colors to ultimately generate white light is tailored on the basis of donor acceptor pair (DAP) recombination mechanism for luminescence. A Q-switched Nd:YAG pulse laser (1064 nm wavelength) was used to carry out the doping experiments. The p and n regions of the white SiC LED were fabricated by laser doping an n-type 6H-SiC and p-type 4H-SiC wafer substrates with respective dopants. Cr, B and Al were used as p-type dopants (acceptors) while N and Se were used as n-type dopants (donors). Deep and shallow donor and acceptor impurity level states formed by these dopants tailor the color properties for pure white light emission. The electromagnetic field of lasers and non-equilibrium doping conditions enable laser doping of SiC with increased dopant diffusivity and enhanced solid solubility. A thermal model is utilized to determine the laser doping parameters for temperature distribution at various depths of the wafer and a diffusion model is presented including the effects of Fick's diffusion, laser electromagnetic field and thermal stresses due to localized laser heating on the mass flux of dopant atoms. The dopant diffusivity is calculated as a function of temperature at different depths of the wafer based on measured dopant concentration profile. The maximum diffusivities achieved in this study are 4.61x10-10 cm2/s at 2898 K and 6.92x10-12 cm2/s at 3046 K for Cr in 6H-SiC and 4H-SiC respectively. Secondary ion mass spectrometric (SIMS) analysis showed the concentration profile of Cr in SiC having a penetration depth ranging from 80 nm in p-type 4H-SiC to 1.5 [micro]m in n-type 6H-SiC substrates respectively. The SIMS data revealed enhanced solid solubility (2.29x1019 cm-3 in 6H-SiC and 1.42x1919 cm-3 in 4H-SiC) beyond the equilibrium limit (3x1017 cm-3 in 6H-SiC above 2500 [degrees]C) for Cr in SiC. It also revealed similar effects for Al and N. The roughness, surface chemistry and crystalline integrity of the doped sample were examined by optical interferometer, energy dispersive X-ray spectrometry (EDS) and transmission electron microscopy (TEM) respectively. Inspite of the larger atomic size of Cr compared to Si and C, the non-equilibrium conditions during laser doping allow effective incorporation of dopant atoms into the SiC lattice without causing any damage to the surface or crystal lattice. Deep Level Transient Spectroscopy (DLTS) confirmed the deep level acceptor state of Cr with activation energies of Ev+0.80 eV in 4H-SiC and Ev+0.45 eV in 6H-SiC. The Hall Effect measurements showed the hole concentration to be 1.98x1019 cm-3 which is almost twice the average Cr concentration (1x1019 cm-3) obtained from the SIMS data. These data confirmed that almost all of the Cr atoms were completely activated to the double acceptor state by the laser doping process without requiring any subsequent annealing step. Electroluminescence studies showed blue (460-498 nm), blue-green (500-520 nm) green (521-575 nm), and orange (650-690 nm) wavelengths due to radiative recombination transitions between donor-acceptors pairs of N-Al, N-B, N-Cr and Cr-Al respectively, while a prominent violet (408 nm) wavelength was observed due to transitions from the nitrogen level to the valence band level. The red (698-738 nm) luminescence was mainly due to metastable mid-bandgap states, however under high injection current it was due to the quantum mechanical phenomenon pertaining to band broadening and overlapping. This RGB combination produced a broadband white light spectrum extending from 380 to 900 nm. The color space tri-stimulus values for 4H-SiC doped with Cr and N were X = 0.3322, Y = 0.3320 and Z = 0.3358 as per 1931 CIE (International Commission on Illumination) corresponding to a color rendering index of 96.56 and the color temperature of 5510 K. And for 6H-SiC n-type doped with Cr and Al, the color space tri-stimulus values are X = 0.3322, Y = 0.3320 and Z = 0.3358. The CCT was 5338 K, which is very close to the incandescent lamp (or black body) and lies between bright midday sun (5200 K) and average daylight (5500 K) while CRI was 98.32. Similar white LED's were also fabricated using Cr, Al, Se as one set of dopants and B, Al, N as another.

Doping in bulk semiconductors (e.g., n- or p- type doping in silicon) allows for precise control of their properties and forms the basis for the development of electronic and photovoltaic devices. Recently, there have been reports on the successful synthesis of doped semiconductor nanocrystals (or quantum dots) for potential applications in solar cells and spintronics. For example, nanocrystals of ZnSe (with zinc-blende lattice structure) and CdSe and ZnO (with wurtzite lattice structure) have been doped successfully with transition-metal (TM) elements (Mn, Co, or Ni). Despite the recent progress, however, the underlying mechanisms of doping in colloidal nanocrystals are not well understood. This thesis reports a comprehensive theoretical analysis toward a fundamental kinetic and thermodynamic understanding of doping in ZnO, CdSe, and ZnSe quantum dots based on first-principles density-functional theory (DFT) calculations. The theoretical predictions of this thesis are consistent with experimental measurements and provide fundamental interpretations for the experimental observations. The mechanisms of doping of colloidal ZnO nanocrystals with the TM elements Mn, Co, and Ni is investigated. The dopant atoms are found to have high binding energies for adsorption onto the Zn-vacancy site of the (0001) basal surface and the O-vacancy site of the (0001) basal surface of ZnO nanocrystals; therefore, these surface vacancies provide viable sites for substitutional doping, which is consistent with experimental measurements. However, the doping efficiencies are affected by the strong tendencies of the TM dopants to segregate at the nanocrystal surface facets, as indicated by the corresponding computed dopant surface segregation energy profiles. Furthermore, using the Mn doping of CdSe as a case study, the effect of nanocrystal size on doping efficiency is explored. It is shown that Mn adsorption onto small clusters of CdSe is characterized by high binding energies, which, in conjunction with the Mn surface segregation characteristics on CdSe nanocrystals, explains experimental reports of high doping efficiency for small-size CdSe clusters. In addition, this thesis presents a systematic analysis of TM doping in ZnSe nanocrystals. The analysis focuses on the adsorption and surface segregation of Mn dopants on ZnSe nanocrystal surface facets, as well as dopant-induced nanocrystal morphological transitions, and leads to a fundamental understanding of the underlying mechanisms of dopant incorporation into growing nanocrystals. Both surface kinetics (dopant adsorption onto the nanocrystal surface facets) and thermodynamics (dopant surface segregation) are found to have a significant effect on the doping efficiencies in ZnSe nanocrystals. The analysis also elucidates the important role in determining the doping efficiency of ZnSe nanocrystals played by the chemical potentials of the growth precursor species, which determine the surface structure and morphology of the nanocrystals.

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In this thesis we delve into the profile doping scandals involving Marion Jones and Lance Armstrong. Our aim is to analyze how the online news media portray doping allegations in sports specifically on these two athletes. Through a textual analysis and approach encompassing framing theory and intersectionality we explore the gender biases that may exist in media coverage and examine the influence of these representations. The connection between media coverage of suspected drug usage and public sentiment was investigated by using methods mentioned above between two fields of sports- cycling and track and field. This research reveals that the choices made by the media when framing their stories about doping shape opinion. This study also underscores the role played on representation by the media on doping crises within sports. It emphasizes the importance of transparent reporting that fosters discussions. By using these findings as a foundation, we can promote fairness, objectivity and evidence-based reporting when addressing instances of doping in sports.  Furthermore, this study contributes to existing literature on how the media portrays doping allegations by providing a framework for examining how these incidents are depicted by media outlets.