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${\mathrm{Zn}\mathrm{Cl}}_2$solutions are promising electrolytes for aqueous zinc-ion batteries. Here, we report a joint computational and experimental study of the structural and dynamic properties of aqueous ${\mathrm{Zn}\mathrm{Cl}}_2$electrolytes with concentrations ranging from salt-in-water to water-in-salt (WIS). By developing a neural network potential (NNP) model, we perform molecular dynamics (MD) simulations with accuracy but at much larger lengths and longer timescales. The NNP predicted structures are validated by the structure factors measured by X-ray total scattering experiments. The MD trajectories provide a comprehensive and quantitative picture of the ${\mathrm{Zn}}^{2+}$solvation shell structures. Additionally, we find that the $\mathrm{O}-\mathrm{H}$covalent bonds in water are strengthened with increasing salt concentration, thus expanding the electrochemical stability window of aqueous electrolytes. In terms of dynamic properties, the calculated and experimentally measured conductivities are in good agreement. Through the analysis of the calculated cation transference number, we propose a three-stage charge carrier transport mechanism with increasing concentration: independent ion transport, strongly correlated ion transport, and small positive charge carrier diffusion through negatively charged polymeric clusters. Our study provides fundamental atomic scale insights into the structure and transport properties of the ${\mathrm{Zn}\mathrm{Cl}}_2$electrolyte that can aid the optimization and development of WIS electrolytes. 

Abstract Wetland hydrologic connections to downstream waters influence stream water quality. However, no systematic approach for characterizing this connectivity exists. Here using physical principles, we categorized conterminous US freshwater wetlands into four hydrologic connectivity classes based on stream contact and flowpath depth to the nearest stream: riparian, non-riparian shallow, non-riparian mid-depth and non-riparian deep. These classes were heterogeneously distributed over the conterminous United States; for example, riparian dominated the south-eastern and Gulf coasts, while non-riparian deep dominated the Upper Midwest and High Plains. Analysis of a national stream dataset indicated acidification and organic matter brownification increased with connectivity. Eutrophication and sedimentation decreased with wetland area but did not respond to connectivity. This classification advances our mechanistic understanding of wetland influences on water quality nationally and could be applied globally. 

In streams macroinvertebrate density and disturbance-sensitive taxa have decreased, and disturbance-tolerant taxa have increased. 

Abstract Watershed resilience is the ability of a watershed to maintain its characteristic system state while concurrently resisting, adapting to, and reorganizing after hydrological (for example, drought, flooding) or biogeochemical (for example, excessive nutrient) disturbances. Vulnerable waters include non-floodplain wetlands and headwater streams, abundant watershed components representing the most distal extent of the freshwater aquatic network. Vulnerable waters are hydrologically dynamic and biogeochemically reactive aquatic systems, storing, processing, and releasing water and entrained (that is, dissolved and particulate) materials along expanding and contracting aquatic networks. The hydrological and biogeochemical functions emerging from these processes affect the magnitude, frequency, timing, duration, storage, and rate of change of material and energy fluxes among watershed components and to downstream waters, thereby maintaining watershed states and imparting watershed resilience. We present here a conceptual framework for understanding how vulnerable waters confer watershed resilience. We demonstrate how individual and cumulative vulnerable-water modifications (for example, reduced extent, altered connectivity) affect watershed-scale hydrological and biogeochemical disturbance response and recovery, which decreases watershed resilience and can trigger transitions across thresholds to alternative watershed states (for example, states conducive to increased flood frequency or nutrient concentrations). We subsequently describe how resilient watersheds require spatial heterogeneity and temporal variability in hydrological and biogeochemical interactions between terrestrial systems and down-gradient waters, which necessitates attention to the conservation and restoration of vulnerable waters and their downstream connectivity gradients. To conclude, we provide actionable principles for resilient watersheds and articulate research needs to further watershed resilience science and vulnerable-water management. 

Abstract Understanding the origin and maintenance of adaptive phenotypic novelty is a central goal of evolutionary biology. However, both hybridization and incomplete lineage sorting can lead to genealogical discordance between the regions of the genome underlying adaptive traits and the remainder of the genome, decoupling inferences about character evolution from population history. Here, to disentangle these effects, we investigated the evolutionary origins and maintenance of Batesian mimicry between North American admiral butterflies (Limenitis arthemis) and their chemically defended model (Battus philenor) using a combination of de novo genome sequencing, whole-genome resequencing, and statistical introgression mapping. Our results suggest that balancing selection, arising from geographic variation in the presence or absence of the unpalatable model, has maintained two deeply divergent color patterning haplotypes that have been repeatedly sieved among distinct mimetic and nonmimetic lineages of Limenitis via introgressive hybridization.