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  3. The earliest evidence of wildfire is documented from two localities: the early mid-Silurian Pen-y-lan Mudstone, Rumney, Wales (UK), and the late Silurian Winnica Formation, Winnica, Poland. Nematophytes dominate both charcoal assemblages. Reflectance data indicate low-temperature fires with localized intense conditions. Fire temperatures are greater in the older and less evolved assemblage. These charcoal assemblages and others, new and previously documented, from the Silurian and earliest Devonian are compared to box models of atmospheric oxygen concentration (pO2). Based on modern charring experiments, these data indicate pO2 is divergent from the broad trends predicted by the COPSE-revisited and GEOCARBSULFOR models. Sustained burnsmore »require a minimum pO2 threshold of 16%, or ~0.75 present atmospheric level. This threshold was first met and, our charcoal data indicate, was exceeded in the mid-Silurian and then, later in the Silurian, attained again repeatedly.« less
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  4. Changes in the geometry and topology of self-assembled membranes underlie diverse processes across cellular biology and engineering. Similar to lipid bilayers, monolayer colloidal membranes have in-plane fluid-like dynamics and out-of-plane bending elasticity. Their open edges and micrometer-length scale provide a tractable system to study the equilibrium energetics and dynamic pathways of membrane assembly and reconfiguration. Here, we find that doping colloidal membranes with short miscible rods transforms disk-shaped membranes into saddle-shaped surfaces with complex edge structures. The saddle-shaped membranes are well approximated by Enneper’s minimal surfaces. Theoretical modeling demonstrates that their formation is driven by increasing the positive Gaussian modulus,more »which in turn, is controlled by the fraction of short rods. Further coalescence of saddle-shaped surfaces leads to diverse topologically distinct structures, including shapes similar to catenoids, trinoids, four-noids, and higher-order structures. At long timescales, we observe the formation of a system-spanning, sponge-like phase. The unique features of colloidal membranes reveal the topological transformations that accompany coalescence pathways in real time. We enhance the functionality of these membranes by making their shape responsive to external stimuli. Our results demonstrate a pathway toward control of thin elastic sheets’ shape and topology—a pathway driven by the emergent elasticity induced by compositional heterogeneity.« less
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  8. Stable glasses (SGs) are formed through surface-mediated equilibration (SME) during physical vapor deposition (PVD). Unlike intermolecular interactions, the role of intramolecular degrees of freedom in this process remains unexplored. Here, using experiments and coarse-grained molecular dynamics simulations, we demonstrate that varying dihedral rotation barriers of even a single bond, in otherwise isomeric molecules, can strongly influence the structure and stability of PVD glasses. These effects arise from variations in the degree of surface mobility, mobility gradients, and mobility anisotropy, at a given deposition temperature ( T dep ). At high T dep , flexible molecules have access to more configurations,more »which enhances the rate of SME, forming isotropic SGs. At low T dep , stability is achieved by out of equilibrium aging of the surface layer. Here, the poor packing of rigid molecules enhances the rate of surface-mediated aging, producing stable glasses with layered structures in a broad range of T dep . In contrast, the dynamics of flexible molecules couple more efficiently to the glass layers underneath, resulting in reduced mobility and weaker mobility gradients, producing unstable glasses. Independent of stability, the flattened shape of flexible molecules can also promote in-plane orientational order at low T dep . These results indicate that small changes in intramolecular relaxation barriers can be used as an approach to independently tune the structure and mobility profiles of the surface layer and, thus, the stability and structure of PVD glasses.« less
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