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Abstract
Spin crossover plays a central role in the structural instability, net magnetic moment modification, metallization, and even in superconductivity in corresponding materials. Most reports on the pressure-induced spin crossover with a large volume collapse have so far focused on compounds with a single transition metal. Here we report a comprehensive high-pressure investigation of a mixed Fe-Mn perovskite La2FeMnO6. Under pressure, the strong coupling between Fe andMn leads to a combined valence/spin transition: Fe3+(S = 5/2) -> Fe2+(S = 0) and Mn3+(S = 2) -> Mn4+(S = 3/2), with an isostructural phase transition. The spin transitions of both Fe and Mn are offset by similar to 20 GPa of the onset pressure, and the lattice collapse occurs in between. Interestingly, Fe3+ ion shows an abnormal behavior when it reaches a lower valence state (Fe2+) accompanied by a +0.5 eV energy shift in the Fe K-absorption edge at 15 GPa. This process is associated with the charge-spin-orbital state transition from high spin Fe3+ to low spin Fe2+, caused by the significantly enhanced t(2g)-e(g) crystal field splitting in the compressed lattice under high pressure. Density functional theory calculations confirm the energy preference of the high-pressure state with charge redistribution accompanied by spin state transition of Fe ions. Moreover, La2FeMnO6 maintains semiconductor behaviors even when the pressure reached 144.5 GPa as evidenced by the electrical transport measurements, despite the huge resistivity decreasing seven orders of magnitude compared with that at ambient pressure. The investigation carried out here demonstrates high flexibility of double perovskites and their good potentials for optimizing the functionality of these materials.
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Abstract
Background: During the acute stroke phase, neutrophils from the peripheral blood are first to arrive in the ischemic brain, which then attracts other immune cells that exacerbate neuroinflammation in the ischemic tissue. Myosin1f was reported to specifically mediate neutrophil migration in the peripheral tissues, but whether it plays a critical role in the neuroinflammatory response after ischemic stroke remains unknown. In this study, we aim to test the hypothesis that myosin1f-mediated neutrophil migration is critical in acute neuroinflammation induced by ischemic stroke.
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Abstract
Runoff in the United States is changing, and this study finds that the measured change is dependent on the geographic region and varies seasonally. Specifically, observed annual total runoff had an insignificant increasing trend in the US between 1950 and 2010, but this insignificance was due to regional heterogeneity with both significant and insignificant increases in the eastern, northern, and southern US, and a greater significant decrease in the western US. Trends for seasonal mean runoff also differed across regions. By region, the season with the largest observed trend was autumn for the east (positive), spring for the north (positive), winter for the south (positive), winter for the west (negative), and autumn for the US as a whole (positive). Based on the detection and attribution analysis using gridded WaterWatch runoff observations along with semi-factorial land surface model simulations from the Multi-scale Synthesis and Terrestrial Model Intercomparison Project (MsTMIP), we found that while the roles of CO2 concentration, nitrogen deposition, and land use and land cover were inconsistent regionally and seasonally, the effect of climatic variations was detected for all regions and seasons, and the change in runoff could be attributed to climate change in summer and autumn in the south and in autumn in the west. We also found that the climate-only and historical transient simulations consistently underestimated the runoff trends, possibly due to precipitation bias in the MsTMIP driver or within the models themselves.
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Abstract
Sodium rhodizonate (Na2C6O6) has very high theoretical capacity as a positive electrode material of sodium-ion batteries, but it still has problems such as low actual capacity and poor electronic/ionic conductivity. In order to improve its conductivity, we investigated its structure and electrical properties under high pressure. By performing in situ X-ray diffraction, Raman, infrared absorption, and alternating current impedance spectroscopy in the range of 0-30 GPa at room temperature, we observed a phase transition at similar to 11 GPa, with the conductivity increasing by an order of magnitude. Above similar to 20 GPa, Na2C6O6 gradually amorphized. During the decompression process, the pressure regulation of the structure and properties of the material are reversible. Our study shows that applying external pressure is an effective tool to improve the conductivity of molecular battery materials. The investigation will help to obtain next-generation electrode materials.
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Abstract
To study systems-level properties of the cell, it is necessary to go beyond individual regulators and target genes to study the regulatory network among transcription factors (TFs). However, it is difficult to directly dissect the TFs mediated genome-wide gene regulatory network (GRN) by experiment. Here, we proposed a hierarchical graphical model to estimate TF activity from mRNA expression by building TF complexes with protein cofactors and inferring TF's downstream regulatory network simultaneously. Then we applied our model on flower development and circadian rhythm processes in Arabidopsis thaliana. The computational results show that the sequence specific bHLH family TF HFR1 recruits the chromatin regulator HAC1 to flower development master regulator TF AG and further activates AG's expression by histone acetylation. Both independent data and experimental results supported this discovery. We also found a flower tissue specific H3K27ac ChIP-seq peak at AG gene body and a HFR1 motif in the center of this H3K27ac peak. Furthermore, we verified that HFR1 physically interacts with HAC1 by yeast two-hybrid experiment. This HFR1-HAC1-AG triplet relationship may imply that flower development and circadian rhythm are bridged by epigenetic regulation and enrich the classical ABC model in flower development. In addition, our TF activity network can serve as a general method to elucidate molecular mechanisms on other complex biological regulatory processes.
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Abstract
A Paris-Edinburgh press combined with a multi-channel collimator assembly has been commissioned at the GeoSoilEnviro Center for Advanced Radiation Sources (GSECARS) beamline for monochromatic X-ray scattering, with an emphasis on studying low-Z liquids, especially silicate liquids at high pressure. The Paris-Edinburgh press is mounted on a general-purpose diffractometer, with a pixel array detector mounted on the detector arm. The incident monochromatic undulator beam with energies up to 60 keV is focused both horizontally and vertically to a beam size about 30 x 30 mu m. With this setup, background scattering from the surrounding pressure media is completely removed at 2 theta angles above 10 degrees for samples larger than 1.05 mm in diameter. Thirty minutes is typically sufficient to collect robust X-ray scattering signals from a 1.6 mm diameter amorphous silicate sample. Cell assemblies for the standard Paris-Edinburgh anvils have been developed and pressures and temperatures up to 7 GPa and 2300 K, respectively, have been maintained steadily over hours. We have also developed a cupped-toroidal Drickamer anvil to further increase pressure and temperature capabilities. The cupped-toroidal Drickamer anvil combines features of a modified Drickamer anvil and the traditional Paris-Edinburgh anvil. Pressures up to 12 GPa have been generated at temperatures up to 2100 K.
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Abstract
Knowledge of the structure in amorphous dioxides is important in many fields of science and engineering. Here we report new experimental results of high-pressure polyamorphism in amorphous TiO2 (a-TiO2). Our data show that the Ti coordination number (CN) increases from 7.2 +/- 0.3 at similar to 16 GPa to 8.8 +/- 0.3 at similar to 70 GPa and finally reaches a plateau at 8.9 +/- 0.3 at less than or similar to 86 GPa. The evolution of the structural changes under pressure is rationalized by the ratio (gamma) of the ionic radius of Ti to that of O. It appears that the CN approximate to 9 plateau correlates with the two 9-fold coordinated polymorphs (cotunnite, Fe2P) with different gamma values. This CN gamma relationship is compared with those of a-SiO2 and a-GeO2, displaying remarkably consistent behavior between CN and gamma. The unified CN-gamma relationship may be generally used to predict the compression behavior of amorphous AO(2) compounds under extreme conditions.
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Abstract
Plant functional traits provide a link in process-based vegetation models between plant-level physiology and ecosystem-level responses. Recent advances in physiological understanding and computational efficiency have allowed for the incorporation of plant hydraulic processes in large-scale vegetation models. However, a more mechanistic representation of water limitation that determines ecosystem responses to plant water stress necessitates a re-evaluation of trait-based constraints for plant carbon allocation, particularly allocation to leaf area. In this review, we examine model representations of plant allocation to leaves, which is often empirically set by plant functional type-specific allometric relationships. We analyze the evolution of the representation of leaf allocation in models of different scales and complexities. We show the impacts of leaf allocation strategy on plant carbon uptake in the context of recent advancements in modeling hydraulic processes. Finally, we posit that deriving allometry from first principles using mechanistic hydraulic processes is possible and should become standard practice, rather than using prescribed allometries. The representation of allocation as an emergent property of scarce resource constraints is likely to be critical to representing how global change processes impact future ecosystem dynamics and carbon fluxes and may reduce the number of poorly constrained parameters in vegetation models.
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Abstract
Combined ultrasonic and X-ray microtomography measurements in situ at high pressure, in conjunction with lattice-Boltzmann simulations, enabled simultaneous investigation several physical parameters including: elastic wave velocities (v(p) and v(s)); apparent Poisson's ratio; pore structure; porosity; and permeability. Experiments were conducted on a simple analog material, porous mold-quality aluminum, in a Paris-Edinburgh cell from 0.14 to 1.36 GPa. Porosity was observed to have a strong inverse dependence on pressure up to similar to 0.9 GPa, while permeability has an anisotropic dependence on pressure. Elastic wave velocity (v(p), v(s)) and apparent Poisson's ratio all increase with pressure, with v(p) agreeing well with the Hashin-Shtrikman upper bound at lower pressures and higher porosities. These results demonstrate a new methodology combining experimental and analytical methods to provide cross-property links between microscopic structure and macroscopic elastic properties. Future investigations on more complex Earth materials may have important implications for our understanding of the composition of the deep Earth.
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Abstract
Where does the carbon released by burning fossil fuels go? Currently, ocean and land systems remove about half of the CO2 emitted by human activities; the remainder stays in the atmosphere. These removal processes are sensitive to feedbacks in the energy, carbon, and water cycles that will change in the future. Observing how much carbon is taken up on land through photosynthesis is complicated because carbon is simultaneously respired by plants, animals, and microbes. Global observations from satellites and air samples suggest that natural ecosystems take up about as much CO2 as they emit. To match the data, our land models generate imaginary Earths where carbon uptake and respiration are roughly balanced, but the absolute quantities of carbon being exchanged vary widely. Getting the magnitude of the flux is essential to make sure our models are capturing the right pattern for the right reasons. Combining two cutting-edge tools, carbonyl sulfide (OCS) and solar-induced fluorescence (SIF), will help develop an independent answer of how much carbon is being taken up by global ecosystems. Photosynthesis requires CO2, light, and water. OCS provides a spatially and temporally integrated picture of the "front door" of photosynthesis, proportional to CO2 uptake and water loss through plant stomata. SIF provides a high-resolution snapshot of the "side door," scaling with the light captured by leaves. These two independent pieces of information help us understand plant water and carbon exchange. A coordinated effort to generate SIF and OCS data through satellite, airborne, and ground observations will improve our process-based models to predict how these cycles will change in the future.
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