Zwitterionic polysaccharides (ZPSs) are exceptional carbohydrates,carrying both positively charged amine groups and negatively chargedcarboxylates, that can be loaded onto MHC-II molecules to... Show moreZwitterionic polysaccharides (ZPSs) are exceptional carbohydrates,carrying both positively charged amine groups and negatively chargedcarboxylates, that can be loaded onto MHC-II molecules to activateT cells. It remains enigmatic, however, how these polysaccharidesbind to these receptors, and to understand the structural featuresresponsible for this "peptide-like" behavior, well-definedZPS fragments are required in sufficient quantity and quality. Wehere present the first total synthesis of Bacteroidesfragilis PS A1 fragments encompassing up to 12 monosaccharides,representing three repeating units. Key to our successful syntheseshas been the incorporation of a C-3,C-6-silylidene-bridged "ring-inverted"galactosamine building block that was designed to act as an apt nucleophileas well as a stereoselective glycosyl donor. Our stereoselective synthesisroute is further characterized by a unique protecting group strategy,built on base-labile protecting groups, which has allowed the incorporationof an orthogonal alkyne functionalization handle. Detailed structuralstudies have revealed that the assembled oligosaccharides take upa bent structure, which translates into a left-handed helix for largerPS A1 polysaccharides, presenting the key positively charged aminogroups to the outside of the helix. The availability of the fragmentsand the insight into their secondary structure will enable detailedinteraction studies with binding proteins to unravel the mode of actionof these unique oligosaccharides at the atomic level. Show less
Increasing knowledge of the impacts of pesticides on soil ecological communities is fundamental to a comprehensive understanding of the functional changes in the global agroecosystem industry. In... Show moreIncreasing knowledge of the impacts of pesticides on soil ecological communities is fundamental to a comprehensive understanding of the functional changes in the global agroecosystem industry. In this study, we examined microbial community shifts in the gut of the soil-dwelling organism Enchytraeus crypticus and functional shifts in the soil microbiome (bacteria and viruses) after 21 d of exposure to difenoconazole, one of the main fungicides in intensified agriculture. Our results demonstrated reduced body weight and increased oxidative stress levels of E. crypticus under difenoconazole treatment. Meanwhile, difenoconazole not only altered the composition and structure of the gut microbial community, but also interfered with the soil-soil fauna microecology stability by impairing the abundance of beneficial bacteria. Using soil metagenomics, we revealed that bacterial genes encoding detoxification and viruses encoding carbon cycle genes exhibited a dependent enrichment in the toxicity of pesticides via metabolism. Taken together, these findings advance the understanding of the ecotoxicological impact of residual difenoconazole on the soil-soil fauna micro-ecology, and the ecological importance of virus-encoded auxiliary metabolic genes under pesticide stress. Show less
Systems with local constraints is a new finding in recent researches on complex systems. The heterogeneous spatial interactions and the temporal dependencies among those numerous units make it... Show moreSystems with local constraints is a new finding in recent researches on complex systems. The heterogeneous spatial interactions and the temporal dependencies among those numerous units make it difficult to describe by traditional statistical physics.These complex structures also make information storage and transmission in it is impossible to describe by the random variables with finite outcomes in the classical information theory. In this thesis, we use the statistical ensemble with local constraints to describe those complex systems with heterogeneous interactions and dependencies. This description also helps us find the new information-theoretical bounds in the systems with local constraints, even when the temporal dependencies among numerous units break the asymptotic equipartition property in the classical information theory.Furthermore, we find that the breaking of ensemble equivalence generally exists in systems with local constraints even without the presence of phase transition, and this ensemble nonequivalence in the systems with local constraints without phase transition can be the same strong as the one that only appears on the boundary of phase transitions caused by the long-range interactions. We also find that this breaking of ensemble equivalence will affect the limit of information storage and transmission in systems with local constraints.These results in this thesis extend our understanding of complex systems and information theory. Show less
Plant physiological and metabolic processes are modulated by rhythmic gene expression in a large part. Meanwhile, plants are also regulated by rhizosphere microorganisms, which are fed by root... Show morePlant physiological and metabolic processes are modulated by rhythmic gene expression in a large part. Meanwhile, plants are also regulated by rhizosphere microorganisms, which are fed by root exudates and provide beneficial functions to their plant host. Whether the biorhythms in plants would transfer to the rhizosphere microbial community is still uncertain and their intricate connection remains poorly understood. Here, we investigated the role of the Arabidopsis circadian clock in shaping the rhizosphere microbial community using wild-type plants and clock mutants (cca1-1 and toc1-101) with transcriptomic, metabolomic and 16S rRNA gene sequencing analysis throughout a 24-h period. Deficiencies of the central circadian clock led to abnormal diurnal rhythms for thousands of expressed genes and dozens of root exudates. The bacterial community failed to follow obvious patterns in the 24-h period, and there was lack of coordination with plant growth in the clock mutants. Our results suggest that the robust rhythmicity of genes and root exudation due to circadian clock in plants is an important driving force for the positive succession of rhizosphere communities, which will feedback on plant development. Show less
