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Abstract Single-molecule localization microscopy (SMLM) breaks the optical diffraction limit by numerically localizing sparse fluorescence emitters to achieve super-resolution imaging. Spectroscopic SMLM or sSMLM further allows simultaneous spectroscopy and super-resolution imaging of fluorescence molecules. Hence, sSMLM can extract spectral features with single-molecule sensitivity, higher precision, and higher multiplexity than traditional multicolor microscopy modalities. These new capabilities enabled advanced multiplexed and functional cellular imaging applications. While sSMLM suffers from reduced spatial precision compared to conventional SMLM due to splitting photons to form spatial and spectral images, several methods have been reported to mitigate these weaknesses through innovative optical design and image processing techniques. This review summarizes the recent progress in sSMLM, its applications, and our perspective on future work. Graphical Abstractmore » « less
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Abstract Magneto‐elastic materials facilitate features such as shape programmability, adaptive stiffness, and tunable strength, which are critical for advances in structural and robotic materials. Magneto‐elastic networks are commonly fabricated by employing hard magnets embedded in soft matrices to constitute a monolithic body. These architected network materials have excellent mechanical properties but damage incurred in extreme loading scenarios are permanent. To overcome this limitation, we present a novel design for elastic bars with permanent fixed dipole magnets at their ends and demonstrate their ability to self‐assemble into magneto‐elastic networks under random vibrations. The magneto‐elastic unit configuration, most notably the orientation of end dipoles, is shown to dictate the self‐assembled network topology, which can range from quasi‐ordered triangular lattices to stacks or strings of particles. Network mechanics are probed with uniaxial tensile tests and design criteria for forming stable lightweight 2D networks are established. It is shown that these magneto‐elastic networks rearrange and break gracefully at their magnetic nodes under large excitations and yet recover their original structure at moderate random excitations. This work paves the way for structural materials that can be self‐assembled and repaired on‐the‐fly with random vibrations, and broadens the applications of magneto‐elastic soft materials.more » « less
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Self-discharge and chemically induced mechanical effects degrade calendar and cycle life in intercalation-based electrochromic and electrochemical energy storage devices. In rechargeable lithium-ion batteries, self-discharge in cathodes causes voltage and capacity loss over time. The prevailing self-discharge model centers on the diffusion of lithium ions from the electrolyte into the cathode. We demonstrate an alternative pathway, where hydrogenation of layered transition metal oxide cathodes induces self-discharge through hydrogen transfer from carbonate solvents to delithiated oxides. In self-discharged cathodes, we further observe opposing proton and lithium ion concentration gradients, which contribute to chemical and structural heterogeneities within delithiated cathodes, accelerating degradation. Hydrogenation occurring in delithiated cathodes may affect the chemo-mechanical coupling of layered cathodes as well as the calendar life of lithium-ion batteries.more » « less
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Transposable elements (TEs) and the silencing machinery of their hosts are engaged in a germline arms-race dynamic that shapes TE accumulation and, therefore, genome size. In animal species with extremely large genomes (>10 Gb), TE accumulation has been pushed to the extreme, prompting the question of whether TE silencing also deviates from typical conditions. To address this question, we characterize TE silencing via two pathways—the piRNA pathway and KRAB-ZFP transcriptional repression—in the male and female gonads of Ranodon sibiricus , a salamander species with a ∼21 Gb genome. We quantify 1) genomic TE diversity, 2) TE expression, and 3) small RNA expression and find a significant relationship between the expression of piRNAs and TEs they target for silencing in both ovaries and testes. We also quantified TE silencing pathway gene expression in R. sibiricus and 14 other vertebrates with genome sizes ranging from 1 to 130 Gb and find no association between pathway expression and genome size. Taken together, our results reveal that the gigantic R. sibiricus genome includes at least 19 putatively active TE superfamilies, all of which are targeted by the piRNA pathway in proportion to their expression levels, suggesting comprehensive piRNA-mediated silencing. Testes have higher TE expression than ovaries, suggesting that they may contribute more to the species’ high genomic TE load. We posit that apparently conflicting interpretations of TE silencing and genomic gigantism in the literature, as well as the absence of a correlation between TE silencing pathway gene expression and genome size, can be reconciled by considering whether the TE community or the host is currently “on the attack” in the arms race dynamic.more » « less
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Abstract One of the most challenging aspects of developing high-energy lithium-based batteries is the structural and (electro)chemical stability of Ni-rich active cathode materials at thermally-abused and prolonged cell cycling conditions. Here, we report in situ physicochemical characterizations to improve the fundamental understanding of the degradation mechanism of charged polycrystalline Ni-rich cathodes at elevated temperatures (e.g., ≥ 40 °C). Using multiple microscopy, scattering, thermal, and electrochemical probes, we decouple the major contributors for the thermal instability from intertwined factors. Our research work demonstrates that the grain microstructures play an essential role in the thermal stability of polycrystalline lithium-based positive battery electrodes. We also show that the oxygen release, a crucial process during battery thermal runaway, can be regulated by engineering grain arrangements. Furthermore, the grain arrangements can also modulate the macroscopic crystallographic transformation pattern and oxygen diffusion length in layered oxide cathode materials.more » « less
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Abstract Mn‐rich cathodes balance performance and sustainability but suffer from limited cyclability due to Mn dissolution and cathode‐to‐anode crosstalk. The Jahn‐Teller (J‐T) effect of Mn3+is often linked to the above phenomena, such as in spinel LiMn2O4. However, in typical voltage ranges, significant Mn3+only appears near the end of discharge, highlighting the need to reassess its role in driving Mn dissolution, structural degradation, and battery performance. Here, the spinel cathode's degree of disorder is tailored to expand the Mn redox range, enabling segmentation into J‐T active and less active voltage ranges. Cycling at segmented voltage windows reveals surface degradation mechanisms with and without the major J‐T effect. Despite a stronger J‐T effect below 3.6 V vs. Li/Li+, Mn dissolution is less significant than above 3.6 V. Expanding the cycling window to 2.0–4.3 V causes severe degradation as the J‐T active range induces a tetragonal phase and Mn2+‐rich surface, driving Mn dissolution and consuming Li‐ion inventory in full cells. Reducing electrolyte acidity minimizes Mn3+disproportionation, enabling a stable dopant‐free Mn‐only cathode with a 250 mAh g−1specific capacity. These findings demonstrate that full cells using Mn‐rich cathodes have the potential to avoid the notorious crosstalk problem through electrolyte engineering.more » « less
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