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Abstract
Global carbon emissions continue to acidify the oceans, motivating growing concern for the ability of coral reefs to maintain net positive calcification rates. Efforts to develop robust relationships between coral reef calcification and carbonate parameters such as aragonite saturation state ((arag)) aim to facilitate meaningful predictions of how reef calcification will change in the face of ocean acidification. Here we investigate natural trends in carbonate chemistry of a coral reef flat over diel cycles and relate these trends to benthic carbon fluxes by quantifying net community calcification and net community production. We find that, despite an apparent dependence of calcification on (arag) seen in a simple pairwise relationship, if the dependence of net calcification on net photosynthesis is accounted for, knowing (arag) does not add substantial explanatory value. This suggests that, over short time scales, the control of (arag) on net calcification is weak relative to factors governing net photosynthesis.
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Abstract
As theoretically hypothesized for several decades in group IV transition metals, we have discovered a dynamically stabilized body-centered cubic (bcc) intermediate state in Zr under uniaxial loading at sub-nanosecond timescales. Under ultrafast shock wave compression, rather than the transformation from alpha-Zr to the more disordered hex-3 equilibrium omega-Zr phase, in its place we find the formation of a previously unobserved nonequilibrium bcc metastable intermediate. We probe the compression-induced phase transition pathway in zirconium using time-resolved sub-picosecond x-ray diffraction analysis at the Linac Coherent Light Source. We also present molecular dynamics simulations using a potential derived from first-principles methods which independently predict this intermediate phase under ultrafast shock conditions. In contrast with experiments on longer timescale (> 10 ns) where the phase diagram alone is an adequate predictor of the crystalline structure of a material, our recent study highlights the importance of metastability and time dependence in the kinetics of phase transformations.
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Abstract
The Earth warms both when fossil fuel carbon is oxidized to carbon dioxide and when greenhouse effect of carbon dioxide inhibits longwave radiation from escaping to space. Various important time scales and ratios comparing these two climate forcings have not previously been quantified. For example, the global and time-integrated radiative forcing from burning a fossil fuel exceeds the heat released upon combustion within 2 months. Over the long lifetime of CO2 in the atmosphere, the cumulative CO2-radiative forcing exceeds the amount of energy released upon combustion by a factor >100,000. For a new power plant, the radiative forcing from the accumulation of released CO2 exceeds the direct thermal emissions in less than half a year. Furthermore, we show that the energy released from the combustion of fossil fuels is now about 1.71% of the radiative forcing from CO2 that has accumulated in the atmosphere as a consequence of historical fossil fuel combustion.
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Abstract
The high-pressure structural and vibrational properties of a layered transition metal dichalcogenide 2H-NbSe2 were investigated using single-crystal x-ray diffraction and Raman spectroscopy, demonstrating its structural stability up to 35 GPa. The lattice compressibility changes character from being highly anisotropic at low pres-sures to largely isotropic at high pressures. Concomitantly, the interatomic bonds demonstrate highly anisotropic compression behavior with the Se-Se interlayer bonds compressing by >20%, while the intramolecular Se-Se distance shows a nonmonotonic pressure dependence with a maximum at-12 GPa. The nearest-neighbor central force lattice vibrational model yields pressure dependencies of the interatomic forces in qualitative agreement with bond length compression, providing insight into the vibrational properties of 2H-NbSe2 at high pressures.
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Abstract
High-pressure chemistry is known to inspire the creation of unexpected new classes of compounds with exceptional properties. Here, we employ the laser-heated diamond anvil cell technique for synthesis of a Dirac material BeN4. A triclinic phase of beryllium tetranitride tr-BeN4 was synthesized from elements at similar to 85 GPa. Upon decompression to ambient conditions, it transforms into a compound with atomic-thick BeN4 layers interconnected via weak van der Waals bonds and consisting of polyacetylene-like nitrogen chains with conjugated pi systems and Be atoms in square-planar coordination. Theoretical calculations for a single BeN4 layer show that its electronic lattice is described by a slightly distorted honeycomb structure reminiscent of the graphene lattice and the presence of Dirac points in the electronic band structure at the Fermi level. The BeN4 layer, i.e., beryllonitrene, represents a qualitatively new class of 2D materials that can be built of a metal atom and polymeric nitrogen chains and host anisotropic Dirac fermions.
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Abstract
The climatic effects of Solar Radiation Management (SRM) geoengineering have been often modeled by simply reducing the solar constant. This is most likely valid only for space sunshades and not for atmosphere and surface based SRM methods. In this study, a global climate model is used to evaluate the differences in the climate response to SRM by uniform solar constant reduction and stratospheric aerosols. Our analysis shows that when global mean warming from a doubling of CO2 is nearly cancelled by both these methods, they are similar when important surface and tropospheric climate variables are considered. However, a difference of 1 K in the global mean stratospheric (61-9.8 hPa) temperature is simulated between the two SRM methods. Further, while the global mean surface diffuse radiation increases by similar to 23 % and direct radiation decreases by about 9 % in the case of sulphate aerosol SRM method, both direct and diffuse radiation decrease by similar fractional amounts (similar to 1.0 %) when solar constant is reduced. When CO2 fertilization effects from elevated CO2 concentration levels are removed, the contribution from shaded leaves to gross primary productivity (GPP) increases by 1.8 % in aerosol SRM because of increased diffuse light. However, this increase is almost offset by a 15.2 % decline in sunlit contribution due to reduced direct light. Overall both the SRM simulations show similar decrease in GPP (similar to 8 %) and net primary productivity (similar to 3 %). Based on our results we conclude that the climate states produced by a reduction in solar constant and addition of aerosols into the stratosphere can be considered almost similar except for two important aspects: stratospheric temperature change and the consequent implications for the dynamics and the chemistry of the stratosphere and the partitioning of direct versus diffuse radiation reaching the surface. Further, the likely dependence of global hydrological cycle response on aerosol particle size and the latitudinal and height distribution of aerosols is discussed.
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Abstract
Polynitrogen molecules are attractive for high-energy-density materials due to energy stored in nitrogen-nitrogen bonds; however, it remains challenging to find energy-efficient synthetic routes and stabilization mechanisms for these compounds. Direct synthesis from molecular dinitrogen requires overcoming large activation barriers and the reaction products are prone to inherent inhomogeneity. Here we report the synthesis of planar N-6(2-) hexazine dianions, stabilized in K2N6, from potassium azide (KN3) on laser heating in a diamond anvil cell at pressures above 45 GPa. The resulting K2N6, which exhibits a metallic lustre, remains metastable down to 20 GPa. Synchrotron X-ray diffraction and Raman spectroscopy were used to identify this material, through good agreement with the theoretically predicted structural, vibrational and electronic properties for K2N6. The N-6(2)-rings characterized here are likely to be present in other high-energy-density materials stabilized by pressure. Under 30 GPa, an unusual N-2(0.75-)-containing compound with the formula K-3(N-2)(4) was formed instead.
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Abstract
Changes in sea ice cover have important consequences for both Earth's energy budget and atmospheric dynamics. Sea ice acts as a positive feedback in the climate system, amplifying effects of radiative forcing while also affecting the meridional and interhemispheric temperature gradients that can impact mid-and low latitude atmospheric circulation. In this study, we partition and evaluate the effects of changing sea ice cover on global warming using a set of simulations with active and suppressed sea ice response. Two aspects of CO2-induced sea ice changes are investigated: (1) the effect of changing sea ice cover on global and local temperature changes; and (2) the impact of sea ice loss on atmospheric circulation and extreme weather events. We find that in the absence of sea ice decline, global temperature response decreases by 21-37%, depending on the sea ice treatment and the CO2 forcing applied. Weakened global warming in the absence of changes in sea ice cover is not only due to a decreased high latitude warming but is also a consequence of a weaker tropical warming. In the northern midlatitudes, sea ice decline affects the magnitude and sign of zonal wind response to global warming in the winter and autumn seasons. Presence or absence of sea ice cover impacts the intensity and frequency of winter extreme precipitation and temperature events (temperature minima, number of heavy precipitation days and number of ice days). For some of the analyzed extreme weather indices, the difference between the responses with and without sea ice decline is eliminated when taking into account the amplifying effect of sea ice loss on hemispheric warming. However, in other cases, we find the influence of higher order factors, exerting weaker but opposing effects than those expected from the global temperature increase.
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Abstract
The response of rapidly compressed highly oriented pyrolytic graphite (HOPG) normal to its basal plane was investigated at a pressure of & SIM;80 GPa. Ultrafast x-ray diffraction using & SIM;100 fs pulses at the Materials Under Extreme Conditions sector of the Linac Coherent Light Source was used to probe the changes in crystal structure resulting from picosecond timescale compression at laser drive energies ranging from 2.5 to 250 mJ. A phase transformation from HOPG to a highly textured hexagonal diamond structure is observed at the highest energy, followed by relaxation to a still highly oriented, but distorted graphite structure following release. We observe the formation of a highly oriented lonsdaleite within 20 ps, subsequent to compression. This suggests that a diffusionless martensitic mechanism may play a fundamental role in phase transition, as speculated in an early work on this system, and more recent static studies of diamonds formed in impact events. Published by AIP Publishing.
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Abstract
The Antarctic Ice Sheet stores water equivalent to 58 m in global sea-level rise. We show in simulations using the Parallel Ice Sheet Model that burning the currently attainable fossil fuel resources is sufficient to eliminate the ice sheet. With cumulative fossil fuel emissions of 10,000 gigatonnes of carbon (GtC), Antarctica is projected to become almost ice-free with an average contribution to sea-level rise exceeding 3 m per century during the first millennium. Consistent with recent observations and simulations, the West Antarctic Ice Sheet becomes unstable with 600 to 800 GtC of additional carbon emissions. Beyond this additional carbon release, the destabilization of ice basins in both West and East Antarctica results in a threshold increase in global sea level. Unabated carbon emissions thus threaten the Antarctic Ice Sheet in its entirety with associated sea-level rise that far exceeds that of all other possible sources.
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