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  1. Sn(II)-based perovskite oxides, being the subject of longstanding theoretical interest for the past two decades, have been synthesized for the first time in the form of nano eggshell particle morphologies. All past reported synthetic attempts have been unsuccessful owing to their metastable nature, i.e. , by their thermodynamic instability towards decomposition to their constituent oxides. A new approach was discovered that finally provides an effective solution to surmounting this intractable synthetic barrier and which can be the key to unlocking the door to many other predicted metastable oxides. A low-melting KSn2Cl5 salt was utilized to achieve a soft topotactic exchange of Sn(II) cations into a Ba-containing perovskite, i.e., BaHfO3 with particle sizes of ∼350 nm, at a low reaction temperature of 200 °C. The resulting particles exhibit nanoshell-over-nanoshell morphologies, i.e., with SnHfO3 forming as ∼20 nm thick shells over the surfaces of the BaHfO3 eggshell particles. Formation of the metastable SnHfO3 is found to be thermodynamically driven by the co-production of the highly stable BaCl2 and KCl side products. Despite this, total energy calculations show that Sn(II) distorts from the A-site asymmetrically and randomly and the interdiffusion has a negligible impact on the energy of the system (i.e., layered vs.more »solid solution). Additionally, nano eggshell particle morphologies of BaHfO3 were found to yield highly pure SnHfO3 for the first time, thus circumventing the intrinsic ion-diffusion limits occurring at this low reaction temperature. In summary, these results demonstrate that the metastability of many theoretically predicted Sn(II)-perovskites can be overcome by leveraging the high cohesive energies of the reactants, the exothermic formation of a stable salt side product, and a shortened diffusion pathway for the Sn(II) cations.« less
    Free, publicly-accessible full text available November 15, 2023
  2. Abstract Background Spawning migrations are a widespread phenomenon among fishes, often occurring in response to environmental conditions prompting movement into reproductive habitats (migratory cues). However, for many species, individual fish may choose not to migrate, and research suggests that conditions preceding the spawning season (migratory primers) may influence this decision. Few studies have provided empirical descriptions of these prior conditions, partly due to a lack of long-term data allowing for robust multi-year comparisons. To investigate how primers and cues interact to shape the spawning migrations of coastal fishes, we use acoustic telemetry data from Common Snook ( Centropomus undecimalis ) in Everglades National Park, Florida, USA. A contingent of Snook migrate between rivers and coastal spawning sites, varying annually in both the proportion of the population that migrates and the timing of migration within the spawning season. However, the specific environmental factors that serve as migratory primers and cues remain unknown. Methods We used eight years of acoustic telemetry data (2012–2019) from 173 tagged Common Snook to investigate how primers and cues influence migratory patterns at different temporal scales. We hypothesize that (1) interannual differences in hydrologic conditions preceding the spawning season contribute to the number of individuals migrating eachmore »year, and (2) specific environmental cues trigger the timing of migrations during the spawning season. We used GLMMs to model both the annual and seasonal migratory response in relation to flow characteristics (water level, rate of change in water level), other hydrologic/abiotic conditions (temperature, salinity), fish size, and phenological cues independent of riverine conditions (photoperiod, lunar cycle). Results We found that the extent of minimum marsh water level prior to migration and fish size influence the proportion of Snook migrating each year, and that high river water level and daily rates of change serve as primary cues triggering migration timing. Conclusion Our findings illustrate how spawning migrations are shaped by environmental factors acting at different temporal scales and emphasize the importance of long-term movement data in understanding these patterns. Research providing mechanistic descriptions of conditions that promote migration and reproduction can help inform management decisions aimed at conserving ecologically and economically important species.« less
    Free, publicly-accessible full text available December 1, 2023
  3. Researchers can improve the ecological validity of brain research by studying humans moving in real-world settings. Recent work shows that dual-layer EEG can improve the fidelity of electrocortical recordings during gait, but it is unclear whether these positive results extrapolate to non-locomotor paradigms. For our study, we recorded brain activity with dual-layer EEG while participants played table tennis, a whole-body, responsive sport that could help investigate visuomotor feedback, object interception, and performance monitoring. We characterized artifacts with time-frequency analyses and correlated scalp and reference noise data to determine how well different sensors captured artifacts. As expected, individual scalp channels correlated more with noise-matched channel time series than with head and body acceleration. We then compared artifact removal methods with and without the use of the dual-layer noise electrodes. Independent Component Analysis separated channels into components, and we counted the number of high-quality brain components based on the fit of a dipole model and using an automated labeling algorithm. We found that using noise electrodes for data processing provided cleaner brain components. These results advance technological approaches for recording high fidelity brain dynamics in human behaviors requiring whole body movement, which will be useful for brain science research.
    Free, publicly-accessible full text available August 1, 2023
  4. Free, publicly-accessible full text available November 1, 2023
  5. Free, publicly-accessible full text available June 27, 2023
  6. Giovannoni, Stephen J. (Ed.)
    ABSTRACT Microbial nitrification is a critical process governing nitrogen availability in aquatic systems. Freshwater nitrifiers have received little attention, leaving many unanswered questions about their taxonomic distribution, functional potential, and ecological interactions. Here, we reconstructed genomes to infer the metabolism and ecology of free-living picoplanktonic nitrifiers across the Laurentian Great Lakes, a connected series of five of Earth’s largest lakes. Surprisingly, ammonia-oxidizing bacteria (AOB) related to Nitrosospira dominated over ammonia-oxidizing archaea (AOA) at nearly all stations, with distinct ecotypes prevailing in the transparent, oligotrophic upper lakes compared to Lakes Erie and Ontario. Unexpectedly, one ecotype of Nitrosospira encodes proteorhodopsin, which could enhance survival under conditions where ammonia oxidation is inhibited or substrate limited. Nitrite-oxidizing bacteria (NOB) “ Candidatus Nitrotoga” and Nitrospira fluctuated in dominance, with the latter prevailing in deeper, less-productive basins. Genome reconstructions reveal highly reduced genomes and features consistent with genome streamlining, along with diverse adaptations to sunlight and oxidative stress and widespread capacity for organic nitrogen use. Our findings expand the known functional diversity of nitrifiers and establish their ecological genomics in large lake ecosystems. By elucidating links between microbial biodiversity and biogeochemical cycling, our work also informs ecosystem models of the Laurentian Great Lakes, a criticalmore »freshwater resource experiencing rapid environmental change. IMPORTANCE Microorganisms play critical roles in Earth’s nitrogen cycle. In lakes, microorganisms called nitrifiers derive energy from reduced nitrogen compounds. In doing so, they transform nitrogen into a form that can ultimately be lost to the atmosphere by a process called denitrification, which helps mitigate nitrogen pollution from fertilizer runoff and sewage. Despite their importance, freshwater nitrifiers are virtually unexplored. To understand their diversity and function, we reconstructed genomes of freshwater nitrifiers across some of Earth’s largest freshwater lakes, the Laurentian Great Lakes. We discovered several new species of nitrifiers specialized for clear low-nutrient waters and distinct species in comparatively turbid Lake Erie. Surprisingly, one species may be able to harness light energy by using a protein called proteorhodopsin, despite the fact that nitrifiers typically live in deep dark water. Our work reveals the unique biodiversity of the Great Lakes and fills key gaps in our knowledge of an important microbial group, the nitrifiers.« less
    Free, publicly-accessible full text available June 28, 2023
  7. The fungus Candida albicans is the most common cause of yeast infections in humans. Like many other disease-causing microbes, it releases several virulent proteins that invade and damage human cells. This includes the peptide candidalysin which has been shown to be crucial for infection. Human cells are surrounded by a protective membrane that separates their interior from their external environment. Previous work showed that candidalysin damages the cell membrane to promote infection. However, how candidalysin does this remained unclear. Similar peptides and proteins cause harm by inserting themselves into the membrane and then grouping together to form a ring. This creates a hole, or ‘pore’, that weakens the membrane and allows other molecules into the cell’s interior. Here, Russell, Schaefer et al. show that candidalysin uses a unique pore forming mechanism to impair the membrane of human cells. A combination of biophysical and cell biology techniques revealed that the peptide groups together to form a chain. This chain of candidalysin proteins then closes in on itself to create a loop structure that can insert into the membrane to form a pore. Once embedded within the membrane, the proteins within the loops rearrange again to make the pores more stable somore »they can cause greater damage. This type of pore formation has not been observed before, and may open up new avenues of research. For instance, researchers could use this information to develop inhibitors that stop candidalysin from forming chains and harming the membranes of cells. This could help treat the infections caused by C. albicans.« less
    Free, publicly-accessible full text available September 29, 2023
  8. Conditional-probability density functional theory (CP-DFT) is a formally exact method for finding correlation energies from Kohn-Sham DFT without evaluating an explicit energy functional. We present details on how to generate accurate exchange-correlation energies for the ground-state uniform gas. We also use the exchange hole in a CP antiparallel spin calculation to extract the high-density limit. We give a highly accurate analytic solution to the Thomas-Fermi model for this problem, showing its performance relative to Kohn-Sham and it may be useful at high temperatures. We explore several approximations to the CP potential. Results are compared to accurate parametrizations for both exchange-correlation energies and holes.
    Free, publicly-accessible full text available April 22, 2023
  9. Free, publicly-accessible full text available June 13, 2023
  10. Free, publicly-accessible full text available April 1, 2023