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    Luminescence and reactivity of a charge-transfer excited iron complex with nanosecond lifetime - Iron’s abundance and rich coordination chemistry are potentially appealing features for photochemical applications. However, the photoexcitable charge-transfer states of most iron complexes are limited by picosecond or subpicosecond deactivation through low-lying metal-centered states, resulting in inefficient electron-transfer reactivity and complete lack of photoluminescence. In this study, we show that octahedral coordination of iron(II...
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    Earth and Moon impact flux increased at the end of the Paleozoic - The terrestrial impact crater record is commonly assumed to be biased, with erosion thought to eliminate older craters, even on stable terrains. Given that the same projectile population strikes Earth and the Moon, terrestrial selection effects can be quantified by using a method to date lunar craters with diameters greater than 10 kilometers and younger than 1 billion years. We found that the impact rate increased by a factor of 2.6 about 290 m...
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    Structural adaptations of photosynthetic complex I enable ferredoxin-dependent electron transfer - Photosynthetic complex I enables cyclic electron flow around photosystem I, a regulatory mechanism for photosynthetic energy conversion. We report a 3.3-angstrom-resolution cryo–electron microscopy structure of photosynthetic complex I from the cyanobacterium Thermosynechococcus elongatus. The model reveals structural adaptations that facilitate binding and electron transfer from the photosynthetic electron carrier ferredoxin. By mimicking...
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    Observation of magnetically tunable Feshbach resonances in ultracold 23Na40K + 40K collisions - Resonances in ultracold collisions involving heavy molecules are difficult to simulate theoretically and have proven challenging to detect. Here we report the observation of magnetically tunable Feshbach resonances in ultracold collisions between potassium-40 (40K) atoms and sodium-23–potassium-40 (23Na40K) molecules in the rovibrational ground state. We prepare the atoms and molecules in various hyperfine levels of their ground states and...
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    A Eu3+-Eu2+ ion redox shuttle imparts operational durability to Pb-I perovskite solar cells - The components with soft nature in the metal halide perovskite absorber usually generate lead (Pb)0 and iodine (I)0 defects during device fabrication and operation. These defects serve as not only recombination centers to deteriorate device efficiency but also degradation initiators to hamper device lifetimes. We show that the europium ion pair Eu3+-Eu2+ acts as the "redox shuttle" that selectively oxidized Pb0 and reduced I0 defects simultaneou...
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    Concise total syntheses of (-)-jorunnamycin A and (-)-jorumycin enabled by asymmetric catalysis - The bis-tetrahydroisoquinoline (bis-THIQ) natural products have been studied intensively over the past four decades for their exceptionally potent anticancer activity, in addition to strong Gram-positive and Gram-negative antibiotic character. Synthetic strategies toward these complex polycyclic compounds have relied heavily on electrophilic aromatic chemistry, such as the Pictet–Spengler reaction, that mimics their biosynthetic pathways. ...
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    An amygdalar neural ensemble that encodes the unpleasantness of pain - Pain is an unpleasant experience. How the brain’s affective neural circuits attribute this aversive quality to nociceptive information remains unknown. By means of time-lapse in vivo calcium imaging and neural activity manipulation in freely behaving mice encountering noxious stimuli, we identified a distinct neural ensemble in the basolateral amygdala that encodes the negative affective valence of pain. Silencing this nociceptive ensemble...
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    Agriculturally dominated landscapes reduce bee phylogenetic diversity and pollination services - Land-use change threatens global biodiversity and may reshape the tree of life by favoring some lineages over others. Whether phylogenetic diversity loss compromises ecosystem service delivery remains unknown. We address this knowledge gap using extensive genomic, community, and crop datasets to examine relationships among land use, pollinator phylogenetic structure, and crop production. Pollinator communities in highly agricultural landscapes c...
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    Flagellar microtubule doublet assembly in vitro reveals a regulatory role of tubulin C-terminal tails - Microtubule doublets (MTDs), consisting of an incomplete B-microtubule at the surface of a complete A-microtubule, provide a structural scaffold mediating intraflagellar transport and ciliary beating. Despite the fundamental role of MTDs, the molecular mechanism governing their formation is unknown. We used a cell-free assay to demonstrate a crucial inhibitory role of the carboxyl-terminal (C-terminal) tail of tubulin in MTD assembly. Removal of...
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    Strain-specific antibody therapy prevents cytomegalovirus reactivation after transplantation - Cytomegalovirus infection is a frequent and life-threatening complication that significantly limits positive transplantation outcomes. We developed preclinical mouse models of cytomegalovirus reactivation after transplantation and found that humoral immunity is essential for preventing viral recrudescence. Preexisting antiviral antibodies decreased after transplant in the presence of graft-versus-host disease and were not replaced, owing to poor...
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    H3K9me3-heterochromatin loss at protein-coding genes enables developmental lineage specification - Gene silencing by chromatin compaction is integral to establishing and maintaining cell fates. Trimethylated histone 3 lysine 9 (H3K9me3)–marked heterochromatin is reduced in embryonic stem cells compared to differentiated cells. However, the establishment and dynamics of closed regions of chromatin at protein-coding genes, in embryologic development, remain elusive. We developed an antibody-independent method to isolate and map compacted ...
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    Cerebellar modulation of the reward circuitry and social behavior - The cerebellum has been implicated in a number of nonmotor mental disorders such as autism spectrum disorder, schizophrenia, and addiction. However, its contribution to these disorders is not well understood. In mice, we found that the cerebellum sends direct excitatory projections to the ventral tegmental area (VTA), one of the brain regions that processes and encodes reward. Optogenetic activation of the cerebello-VTA projections was rewarding...
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    CRISPR-mediated activation of a promoter or enhancer rescues obesity caused by haploinsufficiency - A wide range of human diseases result from haploinsufficiency, where the function of one of the two gene copies is lost. Here, we targeted the remaining functional copy of a haploinsufficient gene using CRISPR-mediated activation (CRISPRa) in Sim1 and Mc4r heterozygous mouse models to rescue their obesity phenotype. Transgenic-based CRISPRa targeting of the Sim1 promoter or its distant hypothalamic enhancer up-regulated its expression from the e...
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    The importance of synthetic chemistry in the pharmaceutical industry - Innovations in synthetic chemistry have enabled the discovery of many breakthrough therapies that have improved human health over the past century. In the face of increasing challenges in the pharmaceutical sector, continued innovation in chemistry is required to drive the discovery of the next wave of medicines. Novel synthetic methods not only unlock access to previously unattainable chemical matter, but also inspire new concepts as to how we ...
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    Prediction of higher-selectivity catalysts by computer-driven workflow and machine learning - Catalyst design in asymmetric reaction development has traditionally been driven by empiricism, wherein experimentalists attempt to qualitatively recognize structural patterns to improve selectivity. Machine learning algorithms and chemoinformatics can potentially accelerate this process by recognizing otherwise inscrutable patterns in large datasets. Herein we report a computationally guided workflow for chiral catalyst selection using chemoinf...
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    Cortical column and whole-brain imaging with molecular contrast and nanoscale resolution - Optical and electron microscopy have made tremendous inroads toward understanding the complexity of the brain. However, optical microscopy offers insufficient resolution to reveal subcellular details, and electron microscopy lacks the throughput and molecular contrast to visualize specific molecular constituents over millimeter-scale or larger dimensions. We combined expansion microscopy and lattice light-sheet microscopy to image the nanoscale ...
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