Recent predictions and experimental observations of high Tc superconductivity in hydrogen-rich materials at very high pressures are driving the search for superconductivity in the vicinity of room temperature. We have developed a novel preparation technique that is optimally suited for megabar pressure syntheses of superhydrides using pulsed laser heating while maintaining the integrity of sample-probe contacts for electrical transport measurements to 200 GPa. We detail the synthesis and characterization, including four-probe electrical transport measurements, of lanthanum superhydride samples that display a significant drop in resistivity on cooling beginning around 260 K and pressures of 190 GPa. Additional measurements on two additional samples synthesized the same way show resistance drops beginning as high as 280 K at these pressures. The drop in resistance at these high temperatures is not observed in control experiments on pure La as well as in partially transformed samples at these pressures, and x-ray diffraction as a function of temperature on the superhydride reveal no structural changes on cooling. We suggest that the resistance drop is a signature of the predicted superconductivity in LaH10 near room temperature, in good agreement with density functional structure search and BCS theory calculations. *
Recent theoretical calculations predict that megabar pressure stabilizes very hydrogen-rich simple compounds having new clathrate-like structures and remarkable electronic properties including room-temperature superconductivity. X-ray diffraction and optical studies demonstrate that superhydrides of lanthanum can be synthesized with La atoms in an fcc lattice at 170 GPa upon heating to about 1000 K. The results match the predicted cubic metallic phase of LaH having cages of thirty-two hydrogen atoms surrounding each La atom. Upon decompression, the fcc-based structure undergoes a rhombohedral distortion of the La sublattice. The superhydride phases consist of an atomic hydrogen sublattice with H-H distances of about 1.1 Å, which are close to predictions for solid atomic metallic hydrogen at these pressures. With stability below 200 GPa, the superhydride is thus the closest analogue to solid atomic metallic hydrogen yet to be synthesized and characterized.
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Two new polyhydrides of calcium have been synthesized at high pressures and high temperatures and characterized by Raman spectroscopy, infrared spectroscopy, and synchrotron X-ray diffraction. Above 20 GPa and 700 K, we synthesize a phase having a monoclinic (C2/m) structure with Ca 2 H 5 composition, which is characterized by a distinctive vibration at 3789 cm −1 at 25 GPa. The observed Raman spectrum is in close agreement with first-principles calculations of a Ca 2 H 5 structure characterized by a lattice containing a central layer of H 2 molecules oriented along the (100) direction. At higher pressures (e.g., 116 GPa and 1600 K), we synthesize another phase, which has the composition of CaH 4 and a denser body-centered tetragonal structure. This weakly metallic phase also contains molecular-like H 2 units, and its spectroscopic as well as diffraction signatures match closely with those predicted from first-principles calculations. This phase is observed to persist on decompression to 60 GPa at room temperature. The elongation of the H−H bond in these hydrides is a result of the Ca−H 2 interaction, analogous to what occurs in molecular compounds, where H 2 binds side-on to a d-element, such as in Kubas complex.
Raman spectroscopic investigations of deuterated gamma-glycine, carried out up to 21 GPa, indicate emergence of a new phase, which is similar to the delta-phase, reported to be formed from the undeuterated gamma-glycine at 3 GPa and the transformation to this phase is complete by 6 GPa. Observed pressure -induced variations in CD2 and N-D stretching modes indicate significant changes in the hydrogen-bonding interactions. Around approximately 15 GPa, splitting of CD2 and C-C stretching modes and discontinuous changes in the slope of CO2 and N-D stretching modes indicate another structural rearrangement across this pressure. The Raman spectra of retrieved phase at ambient conditions suggest that it may be a layered structure similar to the zeta-phase reported to be formed on decompression of the nondeuterated delta-glycine.
The study of hydrogen bonds near symmetrization limit at high pressures is of importance to understand proton dynamics in complex bio-geological processes. We report here the evidence of hydrogen bond symmetrization in the simplest amino acid-carboxylic acid complex, glycinium oxalate, at moderate pressures of 8 GPa using in-situ infrared and Raman spectroscopic investigations combined with first-principles simulations. The dynamic proton sharing between semioxalate units results in covalent-like infinite oxalate chains. At pressures above 12 GPa, the glycine units systematically reorient with pressure to form hydrogen-bonded supramolecular assemblies held together by these chains.
The compression behavior of delafossite compound CuCrO 2 has been investigated by in-situ x-ray diffraction and Raman spectroscopic measurements upto 23.2 and 34 GPa respectively.X-ray diffraction data shows the stability of ambient rhombohedral structure upto ~ 23 GPa.
We report in situ high-pressure Raman spectroscopic as well as X-ray diffraction measurements on bis(glycinium)oxalate, an organic complex of glycine, up to 35 GPa. Several spectral features indicate that at ∼1.7 GPa it transforms to a new structure (phase II) which is characterized by the loss of the center of symmetry and the existence of two nonidentical glycine molecules. Across the transition, all the N-H···O bonds are broken and new weaker N-H···O bonds are formed. Our high-pressure X-ray diffraction studies support the possibility of a non-centrosymmetric space group P2(1) for phase II. Across 5 GPa, another reorganization of N-H···O hydrogen bonds takes place along with a structural transformation to phase III. The C-C stretching mode of oxalate shows pressure-induced softening with large reduction from the initial value of 856 to 820 cm(-1) up to 18 GPa, and further softening is hindered at higher pressures.
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