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  1. We show that the polymer-grafted nanoparticles (NPs) initially welldispersed in a polymer matrix segregate to the free surface of a film upon thermal annealing in the one-phase region of the phase diagram because the grafted polymer has a lower surface energy than the matrix polymer. Using a combination of atomic force microscopy, transmission electron microscopy, and Rutherford backscattering spectrometry, the evolution of the poly(methyl methacrylate)-grafted silica NP (PMMA NP) surface excess in 25/75 wt % PMMA NP/poly(styrene-ranacrylonitrile) films is observed as a function of annealing time at 150 °C (T < TLCST). The temporal growth of the surface excess is interpreted as a competition between entropic contributions, surface energy differences of the constituents, and the Flory−Huggins interaction parameter, χ. For the first time in a miscible polymer nanocomposite mixture, quantitative comparisons of NP surface segregation are made with the predictions of theory derived for analogous polymer blends. These studies provide insight for designing polymer nanocomposite films with advantageous surface properties such as wettability and hardness and motivate the need for developing rigorous models that capture complex polymer nanocomposite phase behaviors.
    Free, publicly-accessible full text available August 23, 2023
  2. abstract Coastal ecosystems play a disproportionately large role in society, and climate change is altering their ecological structure and function, as well as their highly valued goods and services. In the present article, we review the results from decade-scale research on coastal ecosystems shaped by foundation species (e.g., coral reefs, kelp forests, coastal marshes, seagrass meadows, mangrove forests, barrier islands) to show how climate change is altering their ecological attributes and services. We demonstrate the value of site-based, long-term studies for quantifying the resilience of coastal systems to climate forcing, identifying thresholds that cause shifts in ecological state, and investigating the capacity of coastal ecosystems to adapt to climate change and the biological mechanisms that underlie it. We draw extensively from research conducted at coastal ecosystems studied by the US Long Term Ecological Research Network, where long-term, spatially extensive observational data are coupled with shorter-term mechanistic studies to understand the ecological consequences of climate change.
    Free, publicly-accessible full text available August 16, 2023
  3. Abstract Lake ecosystems, as integrators of watershed and climate stressors, are sentinels of change. However, there is an inherent time-lag between stressors and whole-lake response. Aquatic metabolism, including gross primary production (GPP) and respiration (R), of stream–lake transitional zones may bridge the time-lag of lake response to allochthonous inputs. In this study, we used high-frequency dissolved oxygen data and inverse modeling to estimate daily rates of summer epilimnetic GPP and R in a nutrient-limited oligotrophic lake at two littoral sites located near different major inflows and at a pelagic site. We examined the relative importance of stream variables in comparison to meteorological and in-lake predictors of GPP and R. One of the inflow streams was substantially warmer than the other and primarily entered the lake’s epilimnion, whereas the colder stream primarily mixed into the metalimnion or hypolimnion. Maximum GPP and R rates were 0.2–2.5 mg O 2 L −1  day −1 (9–670%) higher at littoral sites than the pelagic site. Ensemble machine learning analyses revealed that > 30% of variability in daily littoral zone GPP and R was attributable to stream depth and stream–lake transitional zone mixing metrics. The warm-stream inflow likely stimulated littoral GPP and R, while the cold-stream inflow only stimulatedmore »littoral zone GPP and R when mixing with the epilimnion. The higher GPP and R observed near inflows in our study may provide a sentinel-of-the-sentinel signal, bridging the time-lag between stream inputs and in-lake processing, enabling an earlier indication of whole-lake response to upstream stressors.« less
    Free, publicly-accessible full text available July 1, 2023
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  6. Free, publicly-accessible full text available February 1, 2023
  7. Abstract Climate models of varying complexity have been used for decades to investigate the impact of mountains on the atmosphere and surface climate. Here, the impact of removing the continental topography on the present-day ocean climate is investigated using three different climate models spanning multiple generations. An idealized study is performed where all present-day land surface topography is removed and the equilibrium change in the oceanic mean state with and without the mountains is studied. When the mountains are removed, changes found in all three models include a weakening of the Atlantic meridional overturning circulation and associated SST cooling in the subpolar North Atlantic. The SSTs also warm in all the models in the western North Pacific Ocean associated with a northward shift of the atmospheric jet and the Kuroshio. In the ocean interior, the magnitude of the temperature and salinity response to removing the mountains is relatively small and the sign and magnitude of the changes generally vary among the models. These different interior ocean responses are likely related to differences in the mean state of the control integrations due to differences in resolution and associated subgrid-scale mixing parameterizations. Compared to the results from 4xCO 2 simulations, the interiormore »ocean temperature changes caused by mountain removal are relatively small; however, the oceanic circulation response and Northern Hemisphere near-surface temperature changes are of a similar magnitude to the response to such radiative forcing changes.« less
    Free, publicly-accessible full text available February 15, 2023
  8. Free, publicly-accessible full text available April 1, 2023
  9. Free, publicly-accessible full text available February 1, 2023
  10. Recently, superhydrides have been computationally identified and subsequently synthesized with a variety of metals at very high pressures. In this work, we evaluate the possibility of synthesizing superhydrides by uniquely combining electrochemistry and applied pressure. We perform computational searches using density functional theory and particle swarm optimization calculations over a broad range of pressures and electrode potentials. Using a thermodynamic analysis, we construct pressure–potential phase diagrams and provide an alternate synthesis concept, pressure–potential (P2), to access phases having high hydrogen content. Palladium–hydrogen is a widely studied material system with the highest hydride phase being Pd3H4. Most strikingly for this system, at potentials above hydrogen evolution and ∼ 300 MPa pressure, we find the possibility to make palladium superhydrides (e.g., PdH10). We predict the generalizability of this approach for La-H, Y-H, and Mg-H with 10- to 100-fold reduction in required pressure for stabilizing phases. In addition, theP2strategy allows stabilizing additional phases that cannot be done purely by either pressure or potential and is a general approach that is likely to work for synthesizing other hydrides at modest pressures.