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Fungal bioluminescence is a fascinating natural process, standing out for the continuous conversion of chemical energy into light. The structure of fungal oxyluciferin (light emitter) was proposed in 2017, being different and more complex than other oxyluciferins. The complexity of fungal oxyluciferin arises from diverse equilibria such as keto/enol tautomerization or deprotonation equilibria of four titratable groups. For this reason, still some crucial details of its structure remain unexplored. To obtain further structural information, a combined experimental and computational study of natural and three synthetic fungal oxyluciferin analogues has been performed. Here, we state the most stable chemical form of fungal oxyluciferin regarding its keto and enol tautomers, in the ground and excited states. We propose the (3Z,5E)-6-(3,4-dihydroxyphenyl)-4-hydroxy-2-oxohexa-3,5-dienoic acid form as the light emitter (fluorescent state) in water solution. Moreover, we show that chemical modifications on fungal oxyluciferin can affect the relative stability of the conformers. Furthermore, we show the clear effect of pH on emission. General conclusions about the role of these titratable groups in emission modulation have been drawn, such as the key role of dihydroxyphenyl deprotonation. This study is key to further analyze the properties of fungal bioluminescence and propose novel synthetic analogues.The continued growth in the demand of data storage and processing has spurred the development of high-performance storage technologies and brain-inspired neuromorphic hardware. Semiconductor quantum dots (QDs) offer an appealing option for these applications since they combine excellent electronic/optical properties and structural stability and can address the requirements of low-cost, large-area, and solution-based manufactured technologies. Here, we focus on the development of nonvolatile memories and neuromorphic computing systems based on QD thin-film solids. We introduce recent advances of QDs and highlight their unique electrical and optical features for designing future electronic devices. We also discuss the advantageous traits of QDs for novel and optimized memory techniques in both conventional flash memories and emerging memristors. Then, we review recent advances in QD-based neuromorphic devices from artificial synapses to light-sensory synaptic platforms. Finally, we highlight major challenges for commercial translation and consider future directions for the postsilicon era.Chitosan (CS), a natural biopolymer, has been extensively explored for multiple applications including tissue engineering, gene therapy, bioimaging, and sewage treatment due to its abundant availability, intrinsic biocompatibility, biodegradability, and tunable biological properties. Nevertheless, the actual use of CS is limited because of its water-insolubility in physiological circumstances, which could be optimized by chemical modifications via active side groups. Etherification is one of the most widely used reactions to obtain water-soluble CS derivatives, such as hydroxybutyl CS (HBC). HBC, synthesized by grafting hydroxybutyl groups to the functional hydroxyl and amino groups of CS skeleton, has been demonstrated to possess superior biological properties over those of CS, especially satisfactory water solubility in neutral condition and reversible stimulus-response against external heat. Meanwhile, the unique characteristics of thermally sensitive "sol-gel" and "sol-micelle" transition have gained tremendous attention, which differ in heterogeneously and homogeneously synthesized HBC. Herein, we discuss the synthesis (heterogeneously and homogeneously) of HBC, favorable physiochemical properties of HBC, and HBC-centered biocomposites in a range of formulations or dosage forms such as sponges, gels, nanoparticles, nanofibers, and films. Meanwhile, we summarize the potential bioapplications and trends of HBC and HBC centered biocomposites and offer our perspectives on the plausible advances in this field in the near future.Cross-linking mass spectrometry (XL-MS) has become a powerful structural tool for defining protein-protein interactions (PPIs) and elucidating architectures of large protein assemblies. To advance XL-MS studies, we have previously developed a series of sulfoxide-containing MS-cleavable cross-linkers to facilitate the detection and identification of cross-linked peptides using multistage mass spectrometry (MSn). While current sulfoxide-based cross-linkers are effective for in vivo and in vitro XL-MS studies at the systems-level, new reagents are still needed to help expand PPI coverage. To this end, we have designed and synthesized six variable-length derivatives of disuccinimidyl sulfoxide (DSSO) to better understand the effects of spacer arm modulation on MS-cleavability, fragmentation characteristics, and MS identification of cross-linked peptides. In addition, the impact on cross-linking reactivity was evaluated. Moreover, alternative MS2-based workflows were explored to determine their feasibility for analyzing new sulfoxide-containing cross-linked products. read more Based on the results of synthetic peptides and a model protein, we have further demonstrated the robustness and predictability of sulfoxide chemistry in designing MS-cleavable cross-linkers. Importantly, we have identified a unique asymmetric design that exhibits preferential fragmentation of cross-links over peptide backbones, a desired feature for MSn analysis. This work has established a solid foundation for further development of sulfoxide-containing MS-cleavable cross-linkers with new functionalities.The modularity of protein domains is well-known, but the existence of independent domains that confer function in RNA is less established. Recently, a family of RNA aptamers termed ykkC was discovered; they bind at least four ligands of very different chemical composition, including guanidine, phosphoribosyl pyrophosphate (PRPP), and guanosine tetraphosphate (ppGpp) (graphical abstract). Structures of these aptamers revealed an architecture characterized by two coaxial helical stacks. The first helix appears to be a generic scaffold, while the second helix forms the most contacts to the ligands. To determine if these two regions within the aptamer are modular units for ligand recognition, we swapped the ligand-binding coaxial stacks of a guanidine aptamer and a PRPP aptamer. This operation, in combination with a single mutation in the scaffold domain, achieved full switching of ligand specificity. This finding suggests that the ligand-binding helix largely dictates the ligand specificity of ykkC RNAs and that the scaffold coaxial stack is generally compatible with various ykkC ligand-binding modules.
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