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  1. Abstract Bacterial natural product biosynthetic genes, canonically clustered, have been increasingly found to rely on hidden enzymes encoded elsewhere in the genome for completion of biosynthesis. The study and application of lanthipeptides are frequently hindered by unclustered protease genes required for final maturation. Here, we establish a global correlation network bridging the gap between lanthipeptide precursors and hidden proteases. Applying our analysis to 161,954 bacterial genomes, we establish 5209 correlations between precursors and hidden proteases, with 91 prioritized. We use network predictions and co-expression analysis to reveal a previously missing protease for the maturation of class I lanthipeptide paenilan. We further discover widely distributed bacterial M16B metallopeptidases of previously unclear biological function as a new family of lanthipeptide proteases. We show the involvement of a pair of bifunctional M16B proteases in the production of previously unreported class III lanthipeptides with high substrate specificity. Together, these results demonstrate the strength of our correlational networking approach to the discovery of hidden lanthipeptide proteases and potentially other missing enzymes for natural products biosynthesis.
    Free, publicly-accessible full text available December 1, 2023
  2. The Beishan orogen is part of the Neoproterozoic to early Mesozoic Central Asian Orogenic System in central Asia that exposes ophiolitic complexes, passive-margin strata, arc assemblages, and Precambrian basement rocks. To better constrain the tectonic evolution of the Beishan orogen, we conducted field mapping, U-Pb zircon dating, whole-rock geochemical analysis, and Sr-Nd isotopic analysis. The new results, when interpreted in the context of the known geological setting, show that the Beishan region had experienced five phases of arc magmatism at ca. 1450−1395 Ma, ca. 1071−867 Ma, ca. 542−395 Ma, ca. 468−212 Ma, and ca. 307−212 Ma. In order to explain the geological, geochemical, and geochronological data from the Beishan region, we present a tectonic model that involves the following five phases of deformation: (1) Proterozoic rifting that separated the North Beishan block from the Greater North China craton that led to the opening of the Beishan Ocean, (2) early Paleozoic north-dipping subduction (ca. 530−430 Ma) of the Beishan oceanic plate associated with back-arc extension followed by collision between the North and South Beishan microcontinental blocks, (3) northward slab rollback of the south-dipping subducting Paleo-Asian oceanic plate at ca. 450−440 Ma along the northern margin of the North Beishan block thatmore »led to the formation of a northward-younging extensional continental arc (ca. 470−280 Ma) associated with bimodal igneous activity, which indicates that the westward extension of the Solonker suture is located north of the Hongshishan-Pengboshan tectonic zone, (4) Late Carboniferous opening and Permian north-dipping subduction of the Liuyuan Ocean in the southern Beishan orogen, and (5) Mesozoic-Cenozoic intracontinental deformation induced by the final closure of the Paleo-Asian Ocean system in the north and the Tethyan Ocean system in the south.« less
    Free, publicly-accessible full text available July 6, 2023
  3. Triarylmethanols are well-known core structures in natural products and pharmacologically relevant compounds. In general, transition metal-based catalysts or highly reactive organometallics are employed for the synthesis of these compounds. Herein, we report the regioselective tandem C(sp 3 )–H arylation/oxidation of diarylmethanes with nitroarenes to generate arylated alcohols. The present method is general, mild, green, and conducted in air at room temperature. Furthermore, use of triarylmethanes as pro-nucleophiles provides straightforward access to select tetraarylmethanes through a cross-dehydrogenative coupling process.
    Free, publicly-accessible full text available July 12, 2023
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  7. Free, publicly-accessible full text available November 14, 2022
  8. We propose and experimentally demonstrate an optical pulse sampling method for photonic blind source separation. The photonic system processes and separates wideband signals based on the statistical information of the mixed signals, and thus the sampling frequency can be orders of magnitude lower than the bandwidth of the signals. The ultra-fast optical pulses collect samples of the signals at very low sampling rates, and each sample is short enough to maintain the statistical properties of the signals. The low sampling frequency reduces the workloads of the analog to digital conversion and digital signal processing systems. In the meantime, the short pulse sampling maintains the accuracy of the sampled signals, so the statistical properties of the under-sampled signals are the same as the statistical properties of the original signals. The linear power range measurement shows that the sampling system with ultra-narrow optical pulse achieves a 30dB power dynamic range.
    Free, publicly-accessible full text available January 1, 2023
  9. Free, publicly-accessible full text available December 1, 2022
  10. The Proterozoic−Phanerozoic tectonic evolution of the Qilian Shan, Qaidam Basin, and Eastern Kunlun Range was key to the construction of the Asian continent, and understanding the paleogeography of these regions is critical to reconstructing the ancient oceanic domains of central Asia. This issue is particularly important regarding the paleogeography of the North China-Tarim continent and South China craton, which have experienced significant late Neoproterozoic rifting and Phanerozoic deformation. In this study, we integrated new and existing geologic field observations and geochronology across northern Tibet to examine the tectonic evolution of the Qilian-Qaidam-Kunlun continent and its relationships with the North China-Tarim continent to the north and South China craton to the south. Our results show that subduction and subsequent collision between the Tarim-North China, Qilian-Qaidam-Kunlun, and South China continents occurred in the early Neoproterozoic. Late Neoproterozoic rifting opened the North Qilian, South Qilian, and Paleo-Kunlun oceans. Opening of the South Qilian and Paleo-Kunlun oceans followed the trace of an early Neoproterozoic suture. The opening of the Paleo-Kunlun Ocean (ca. 600 Ma) occurred later than the opening of the North and South Qilian oceans (ca. 740−730 Ma). Closure of the North Qilian and South Qilian oceans occurred in the Early Silurian (ca.more »440 Ma), whereas the final consumption of the Paleo-Kunlun Ocean occurred in the Devonian (ca. 360 Ma). Northward subduction of the Neo-Kunlun oceanic lithosphere initiated at ca. 270 Ma, followed by slab rollback beginning at ca. 225 Ma evidenced in the South Qilian Shan and at ca. 194 Ma evidenced in the Eastern Kunlun Range. This tectonic evolution is supported by spatial trends in the timing of magmatism and paleo-crustal thickness across the Qilian-Qaidam-Kunlun continent. Lastly, we suggest that two Greater North China and South China continents, located along the southern margin of Laurasia, were separated in the early Neoproterozoic along the future Kunlun-Qinling-Dabie suture.« less
    Free, publicly-accessible full text available December 24, 2022