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Abstract
Understanding of recently reported putative close-to-room-temperature superconductivity in C-S-H compounds at 267 GPa demands a reproducible synthesis protocol as well as knowledge of the compounds' structure and composition. We synthesized C-S-H compounds with various carbon compositions at high pressures from elemental carbon C and methane CH4, sulfur S, and molecular hydrogen H-2. Here, we focus on compounds synthesized using methane as these allow a straightforward determination of their structure and composition by combining single-crystal x-ray diffraction and Raman spectroscopy. We applied a two-stage synthesis of [(CH4)(x)(H2S)((1-x))](2)H-2 compounds with various compositions by first reacting sulfur and mixed methane-hydrogen fluids and forming CH4-doped H2S crystals at 0.5-3 GPa and then by growing single crystals of the desired hydrogen-rich compound. Raman spectroscopy applied to this material shows the presence of CH4 molecules incorporated into the lattice and allows the determination of the CH4 content, while single-crystal x-ray diffraction results suggest that the methane molecules substitute H2S molecules. The structural behavior of these compounds is very similar to the previously investigated methane-free crystals demonstrating a transition from Al2Cu type I4/mcm molecular crystal to a modulated molecular structure at 20-30 GPa and back to the same basic I4/mcm structure in an extended modification with greatly modified Raman spectra. This latter phase demonstrates a distortion into a Pnma structure at 132-159 GPa and then transforms into a common I m 3 over bar m H3S phase at higher pressures; however, no structural anomaly is detected near 220 GPa, where a sharp upturn in T-c has been reported.
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Abstract
The thermal conductivities of materials are extremely important for many practical applications, such as in understanding the thermal balance and history of the Earth, energy conversion of devices and thermal management of electronics. However, measurements of the thermal conductivity of materials under pressure and understanding of associated thermal transport mechanisms remain some of the most difficult challenges and complex topics in high-pressure research. Breakthroughs in high-pressure experimental techniques enable in situ measurements of thermal conductivity at extreme pressure-temperature conditions. This new capability provides not only a unique insight to understand thermal transport mechanisms in materials but also opportunities to realize reversible modulation of materials' thermal properties. In this Review, we discuss recent progresses in characterization techniques developed at high pressures, in the determination of the thermal conductivity of gases, liquids and solids, as well as in establishing the correlated thermal transport mechanisms. In addition, we focus on the applications of high-pressure and high-temperature experimental simulations of materials in the Earth's interior.
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Abstract
The electronic structure near the Fermi surface determines the electrical properties of the materials, which can be effectively tuned by external pressure. Bi0.5Sb1.5Te3 is a p-type thermoelectric material which holds the record high figure of merit at room temperature. Here it is examined whether the figure of merit of this model system can be further enhanced through some external parameter. With the application of pressure, it is surprisingly found that the power factor of this material exhibits lambda behavior with a high value of 4.8 mW m(-1) K-2 at pressure of 1.8 GPa. Such an enhancement is found to be driven by pressure-induced electronic topological transition, which is revealed by multiple techniques. Together with a low thermal conductivity of about 0.89 W m(-1) K-1 at the same pressure, a figure of merit of 1.6 is achieved at room temperature. The results and findings highlight the electronic topological transition as a new route for improving the thermoelectric properties.
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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 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
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
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 Earth has been releasing vast amounts of heat from deep Earth's interior to the surface since its formation, which primarily drives mantle convection and a number of tectonic activities. In this heat transport process the core-mantle boundary where hot molten core is in direct contact with solid-state mantle minerals has played an essential role to transfer thermal energies of the core to the overlying mantle. Although the dominant heat transfer mechanisms at the lowermost mantle is believed to be both conduction and radiation of the primary lowermost mantle mineral, bridgmanite, the radiative thermal conductivity of bridgmanite has so far been poorly constrained. Here we revealed the radiative thermal conductivity of bridgmanite at core-mantle boundary is substantially high approaching to similar to 5.3 +/- 1.2 W/mK based on newly established optical absorption measurement of single-crystal bridgmanite performed in situ under corresponding deep lower mantle conditions. We found the bulk thermal conductivity at core-mantle boundary becomes similar to 1.5 times higher than the conventionally assumed value, which supports higher heat flow from core, hence more vigorous mantle convection than expected. Results suggest the mantle is much more efficiently cooled, which would ultimately weaken many tectonic activities driven by the mantle convection more rapidly than expected from conventionally believed thermal conduction behavior. (C) 2021 The Author(s). Published by Elsevier B.V.
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Abstract
Searching for new bioactive metabolites from the bacterial genus Streptomyces is a challenging task. Combined genomic tools and metabolomic screening of Streptomyces spp. native to extreme environments could be a promising strategy to discover novel compounds. While Streptomyces of desertic origin have been proposed as a source of new metabolites, their genome mining, phylogenetic analysis, and metabolite profiles to date are scarcely documented. Here, we hypothesized that Streptomyces species of desert environments have evolved with unique biosynthetic potential. To test this, along with an extensive characterization of biosynthetic potential of a desert isolate Streptomyces sp. SAJ15, we profiled phylogenetic relationships among the closest and previously reported Streptomyces of desert origin. Results revealed that Streptomyces strains of desert origin are closer to each other and relatively distinct from Streptomyces of other environments. The draft genome of strain SAJ15 was 8.2 Mb in size, which had 6972 predicted genes including 3097 genes encoding hypothetical proteins. Successive genome mining and phylogenetic analysis revealed the presence of putative novel biosynthetic gene clusters (BGCs) with low incidence in another Streptomyces. In addition, high-resolution metabolite profiling indicated the production of arylpolyene, terpenoid, and macrolide compounds in an optimized medium by strain SAJ15. The relative abundance of different BGCs in arid Streptomyces differed from the non-arid counterparts. Collectively, the results suggested a distinct evolution of desert Streptomyces with a unique biosynthetic potential.
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Abstract
Water availability plays a critical role in shaping terrestrial ecosystems, particularly in low- and mid-latitude regions. The sensitivity of vegetation growth to precipitation strongly regulates global vegetation dynamics and their responses to drought, yet sensitivity changes in response to climate change remain poorly understood. Here we use long-term satellite observations combined with a dynamic statistical learning approach to examine changes in the sensitivity of vegetation greenness to precipitation over the past four decades. We observe a robust increase in precipitation sensitivity (0.624% yr(-1)) for drylands, and a decrease (-0.618% yr(-1)) for wet regions. Using model simulations, we show that the contrasting trends between dry and wet regions are caused by elevated atmospheric CO2 (eCO(2)). eCO(2) universally decreases the precipitation sensitivity by reducing leaf-level transpiration, particularly in wet regions. However, in drylands, this leaf-level transpiration reduction is overridden at the canopy scale by a large proportional increase in leaf area. The increased sensitivity for global drylands implies a potential decrease in ecosystem stability and greater impacts of droughts in these vulnerable ecosystems under continued global change.
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