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Register a new userMetallic Hydrogen Sublattice and Proton Mobility in Copper Hydride at High Pressure
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Added by
Thomas Meier Dr. rer. nat.
Publication date
2020
fields
Physics
and research's language is
English
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Atomic and electronic structures of Cu2H and CuH have been investigated by high pressure NMR spectroscopy, X-ray diffraction and ab-initio calculations. Metallic Cu2H was synthesized at a pressure of 40 GPa, and semi-metallic CuH at 90 GPa, found stable up to 160 GPa. Experiments and computations suggest the formation of a metallic 1H-sublattice as well as a high 1H mobility of ~10-7 cm2/s in Cu2H. Comparison of Cu2H and FeH data suggests that deviations from Fermi gas behavior, formation of conductive hydrogen networks, and high 1H mobility could be common features of metal hydrides.
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Knowledge of the behavior of hydrogen in metal hydrides is the key for understanding their electronic properties. So far, no experimental methods exist to access these properties beyond 100 GPa, where high-Tc superconductivity emerges. Here, we present an 1H-NMR study of cubic FeH up to 200GPa. We observe a distinct deviation from the ideal metallic behavior between 64 and 110 GPa that suggests pressure-induced H-H interactions. Accompanying ab-initio calculations support this interpretation, as they reveal the formation of an intercalating sublattice of electron density, which enhances the hydrogen contribution to the electronic density of states at the Fermi level. This study shows that pressure induced H-H interactions can occur in metal hydrides at much lower compression and larger H-H distances than previously thought and stimulates an alternative pathway in the search for novel high-temperature superconductors.
Hydrogen as a fuel can be stored safely with high volumetric density in metals. It can, however, also be detrimental to metals causing embrittlement. Understanding fundamental behavior of hydrogen at atomic scale is key to improve the properties of metal-metal hydride systems. However, currently, there is no robust technique capable of visualizing hydrogen atoms. Here, we demonstrate that hydrogen atoms can be imaged unprecedentedly with integrated differential phase contrast, a recently developed technique performed in a scanning transmission electron microscope. Images of the titanium-titanium monohydride interface reveal remarkable stability of the hydride phase, originating from the interplay between compressive stress and interfacial coherence. We also uncovered, thirty years after three models were proposed, which one describes the position of the hydrogen atoms with respect to the interface. Our work enables novel research on hydrides and is extendable to all materials containing light and heavy elements, including oxides, nitrides, carbides and borides.
X-ray diffraction and Raman scattering measurements, and first-principles calculations are performed to search for the formation of NaCl-hydrogen compound. When NaCl and H$_{2}$ mixture is laser-heated to above 1500 K at pressures exceeding 40 GPa, we observed the formation of NaClH$_{textit{x}}$ with $textit{P}$6$_{3}$/$textit{mmc}$ structure which accommodates H$_{2}$ molecules in the interstitial sites of NaCl lattice forming ABAC stacking. Upon the decrease of pressure at 300 K, NaClH$_textit{x}$ remains stable down to 17 GPa. Our calculations suggest the observed NaClH$_{textit{x}}$ is NaCl(H$_{2}$). Besides, a hydrogen-richer phase NaCl(H$_{2}$)$_{4}$ is predicted to become stable at pressures above 40 GPa.
At present, hydrogen-based compounds constitute one of the most promising classes of materials for applications as a phonon-mediated high-temperature superconductors. Herein, the behavior of the superconducting phase in tellurium hydride (HTe) at high pressure ($p=300$ GPa) is analyzed in details, by using the isotropic Migdal-Eliashberg equations. The chosen pressure conditions are considered here as a case study which corresponds to the highest critical temperature value ($T_{c}$) in the analyzed material, as determined within recent density functional theory simulations. It is found that the Migdal-Eliashberg formalism, which constitutes a strong-coupling generalization of the Bardeen-Cooper-Schrieffer (BCS) theory, predicts that the critical temperature value ($T_{c}=52.73$ K) is higher than previous estimates of the McMillan formula. Further investigations show that the characteristic dimensionless ratios for the the thermodynamic critical field, the specific heat for the superconducting state, and the superconducting band gap exceeds the limits of the BCS theory. In this context, also the effective electron mass is not equal to the bare electron mass as provided by the BCS theory. On the basis of these findings it is predicted that the strong-coupling and retardation effects play pivotal role in the superconducting phase of HTe at 300 GPa, in agreement with similar theoretical estimates for the sibling hydrogen and hydrogen-based compounds. Hence, it is suggested that the superconducting state in HTe cannot be properly described within the mean-field picture of the BCS theory.
Various tin hydrides SnHx (x = 4, 8, 12, 14) have been theoretically predicted to be stable at high pressures and to show high-critical-temperature superconductivity with Tc ranging from about 70 to 100 K. However, experimental verifications for any of these phases are still lacking to date. Here, we report on the in-situ synthesis, electrical resistance, and synchrotron x-ray diffraction measurements of SnHx at ~ 200 GPa. The main phase of the obtained sample can be indexed with the monoclinic C2/m SnH12 via comparison with the theoretical structural modes. A sudden drop of resistance and the systematic downward shift under external magnetic fields signals the occurrence of superconductivity in SnHx at Tc = ~ 70 K with an upper critical field u0Hc2(0) = ~ 11.2 T, which is relatively low in comparison with other reported high-Tc superhydrides. Various characteristic superconducting parameters are estimated based on the BCS theory.
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