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  1. Abstract Constraining the accommodation, distribution, and circulation of hydrogen in the Earth's interior is vital to our broader understanding of the deep Earth due to the significant influence of hydrogen on the material and rheological properties of minerals. Recently, a great deal of attention has been paid to the high-pressure polymorphs of FeOOH (space groups P21nm and Pnnm). These structures potentially form a hydrogen-bearing solid solution with AlOOH and phase H (MgSiO4H2) that may transport water (OH–) deep into the Earth's lower mantle. Additionally, the pyrite-type polymorph (space group Pa3 of FeOOH), and its potential dehydration have been linked to phenomena as diverse as the introduction of hydrogen into the outer core (Nishi et al. 2017), the formation of ultralow-velocity zones (ULVZs) (Liu et al. 2017), and the Great Oxidation Event (Hu et al. 2016). In this study, the high-pressure evolution of FeOOH was re-evaluated up to ~75 GPa using a combination of synchrotron-based X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FTIR), and optical absorption spectroscopy. Based on these measurements, we report three principal findings: (1) pressure-induced changes in hydrogen bonding (proton disordering or hydrogen bond symmetrization) occur at substantially lower pressures in ε-FeOOH than previously reported and are unlikelymore »to be linked to the high-spin to low-spin transition; (2) ε-FeOOH undergoes a 10% volume collapse coincident with an isostructural Pnnm → Pnnm transition at approximately 45 GPa; and (3) a pressure-induced band gap reduction is observed in FeOOH at pressures consistent with the previously reported spin transition (40 to 50 GPa).« less
  2. The Earth’s mantle transition zone (MTZ) is often considered an internal reservoir for water because its major minerals wadsleyite and ringwoodite can store several oceans of structural water. Whether it is a hydrous layer or an empty reservoir is still under debate. Previous studies suggested the MTZ may be saturated with iron metal. Here we show that metallic iron reacts with hydrous wadsleyite under the pressure and temperature conditions of the MTZ to form iron hydride or molecular hydrogen and silicate with less than tens of parts per million (ppm) water, implying that water enrichment is incompatible with iron saturation in the MTZ. With the current estimate of water flux to the MTZ, the iron metal preserved from early Earth could transform a significant fraction of subducted water into reduced hydrogen species, thus limiting the hydration of silicates in the bulk MTZ. Meanwhile, the MTZ would become gradually oxidized and metal depleted. As a result, water-rich region can still exist near modern active slabs where iron metal was consumed by reaction with subducted water. Heterogeneous water distribution resolves the apparent contradiction between the extreme water enrichment indicated by the occurrence of hydrous ringwoodite and ice VII in superdeep diamonds andmore »the relatively low water content in bulk MTZ silicates inferred from electrical conductivity studies.« less
  3. Atomically thin diamond, also called diamane, is a two-dimensional carbon allotrope and has attracted considerable scientific interest because of its potential physical properties. However, the successful synthesis of a pristine diamane has up until now not been achieved. We demonstrate the realization of a pristine diamane through diamondization of mechanically exfoliated few-layer graphene via compression. Resistance, optical absorption, and X-ray diffraction measurements reveal that hexagonal diamane (h-diamane) with a bandgap of 2.8 ± 0.3 eV forms by compressing trilayer and thicker graphene to above 20 GPa at room temperature and can be preserved upon decompression to ∼1.0 GPa. Theoretical calculations indicate that a (−2110)-oriented h-diamane is energetically stable and has a lower enthalpy than its few-layer graphene precursor above the transition pressure. Compared to gapless graphene, semiconducting h-diamane offers exciting possibilities for carbon-based electronic devices.
  4. Sub-Neptunes are common among the discovered exoplanets. However, lack of knowledge on the state of matter inH2O-rich setting at high pressures and temperatures (PT) places important limitations on our understanding of this planet type. We have conducted experiments for reactions betweenSiO2andH2O as archetypal materials for rock and ice, respectively, at highPT. We found anomalously expanded volumes of dense silica (up to 4%) recovered from hydrothermal synthesis above ∼24 GPa where theCaCl2-type (Ct) structure appears at lower pressures than in the anhydrous system. Infrared spectroscopy identified strong OH modes from the dense silica samples. Both previous experiments and our density functional theory calculations support up to 0.48 hydrogen atoms per formula unit of (Si1xH4x)O2(x=0.12). At pressures above 60 GPa,H2O further changes the structural behavior of silica, stabilizing a niccolite-type structure, which is unquenchable. From unit-cell volume and phase equilibrium considerations, we infer that the niccolite-type phase may contain H with an amount at least comparable with or higher than that of the Ct phase. Our results suggest that the phases containing both hydrogen and lithophile elements could bemore »the dominant materials in the interiors of water-rich planets. Even for fully layered cases, the large mutual solubility could make the boundary between rock and ice layers fuzzy. Therefore, the physical properties of the new phases that we report here would be important for understanding dynamics, geochemical cycle, and dynamo generation in water-rich planets.

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  5. Graphene-based nanodevices have been developed rapidly and are now considered a strong contender for postsilicon electronics. However, one challenge facing graphene-based transistors is opening a sizable bandgap in graphene. The largest bandgap achieved so far is several hundred meV in bilayer graphene, but this value is still far below the threshold for practical applications. Through in situ electrical measurements, we observed a semiconducting character in compressed trilayer graphene by tuning the interlayer interaction with pressure. The optical absorption measurements demonstrate that an intrinsic bandgap of 2.5 ± 0.3 eV could be achieved in such a semiconducting state, and once opened could be preserved to a few GPa. The realization of wide bandgap in compressed trilayer graphene offers opportunities in carbon-based electronic devices.