Design and development of novel one-step reactions that produce nitrogen-containing scaffolds is an invaluable area of chemistry due to the abundance of these moieties in natural products and biologically active molecules. Discovering novel methods using uncommon substrates and rare earth metals to access these significant scaffolds present a challenge. Over the course of my doctoral studies, I have designed, developed and optimized novel reactions by using rarely known substrates and rare earth metals that have afforded important nitrogen-containing scaffolds. The products obtained allow access to otherwise long-to-synthesize molecules and expeditious construction of biologically active molecules.

In this dissertation, we study the most important microscopic aspects that grant molecules such as Single Molecule Magnets (SMMs) their preferential spin direction. We do so by proposing and solving a model that includes correlations between electrons occupying atomic orbitals. In addition, we study the relation between the non-equilibrium electronic transport signatures in a SMM model weakly coupled to a three-terminal single electron transistor device, and the interference features of the SMM model in the presence of a magnetic field. Finally, we investigate the equilibrium transport features in a giant-spin model of a SMM in the Kondo regime. We study how the magnetic field modulation of the energy in a highly anisotropic molecule can affect the conductance of the molecule in the Kondo regime.

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京都大学 / 新制・課程博士 / 博士(医学) / 甲第23806号 / 医博第4852号 / 新制||医||1058(附属図書館) / 京都大学大学院医学研究科医学専攻 / (主査)教授 森信 暁雄, 教授 上野 英樹, 教授 椛島 健治 / 学位規則第4条第1項該当 / Doctor of Medical Science / Kyoto University / DFAM

<p>Secondary metabolites are vital to human health and strategies to improve their production and detection are equally essential. The blue pigmented metabolite actinorhodin produced by <em>Streptomyces coelicolor</em>, a genus renowned for their diverse secondary metabolites, provides a unique opportunity to identify small molecules probes of secondary metabolism. Small molecules capable of altering secondary metabolism will have widespread application in the streptomycetes due to their ease of addition to any culture condition. Taking advantage of the phenotypic versatility of the <em>S. coelicolor</em> lifecycle, we extended our search for small molecule modulators further to include the entire developmental process. In addition to alterations in secondary metabolism, these processes include growth inhibition, precocious sporulation and alterations in aerial hyphae formation and sporulation. This work provides the foundation for studying <em>Streptomyces</em> by chemical manipulation. Those compounds which stimulate secondary metabolism were narrowed down to 19 ARCs (for antibiotic remodeling compounds). From these, a set of 4 structurally related molecules, the ARC2 series, was identified as weak inhibitors of fatty acid biosynthesis and most likely lead to alterations in secondary metabolism through shifting precursors from primary to secondary metabolism. Consistent with the conservation of fatty acid biosynthesis within bacteria, the effect of the ARC2 series extends in general to the actinomycetes. This provides a simple strategy to alter the secondary metabolic profiles of a diverse range of actinomycetes.</p> / Doctor of Philosophy (PhD)