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Register a new userSynthesis of clathrate cerium superhydride CeH9 below 100 GPa with atomic hydrogen sublattice
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Hydrogen-rich superhydrides are believed to be very promising high-Tc superconductors as they are expected to mimic characteristics of metallic hydrogen. Recent experiments discovered superhydrides at very high pressures, e.g. FeH5 at 130 GPa and LaH10 at 170 GPa. With the motivation of discovering new hydrogen-rich high-Tc superconductors at lowest possible pressure, here we report the prediction and experimental synthesis of cerium superhydride CeH9 below 100 GPa in the laser-heated diamond anvil cell. Ab-initio calculations were carried to evaluate the detailed chemistry of the Ce-H system and to understand the structure, stability and superconductivity of CeH9. CeH9 crystallizes in a P63/mmc clathrate structure with a substantially dense 3-dimensional hydrogen sublattice at 100 GPa. These findings shed a new light on the search for superhydrides in close proximity with atomic hydrogen within a feasible pressure range. Discovery of superhydride CeH9 provides a practical platform to further investigate and understand conventional superconductivity in hydrogen rich superhydrides.
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Boron-based clathrate materials, typically with three-dimensional networks of B atoms, have tunable properties through substitution of guest atoms, but the tuning of B cages themselves has not yet been developed. By combining crystal structural search with the laser-heated diamond anvil cell technique, we successfully synthesized a new B-based clathrate boride, LaB8, at ~108 GPa and ~2100 K. The novel structure has a B-richest cage, with 26 B atoms encapsulating a single La atom. LaB8 demonstrates phonon-mediated superconductivity with an estimated transition temperature of 14 K at ambient pressure, mainly originating from electron-phonon coupling of B cage. This work creates a prototype platform for subsequent investigation on tunable electronic properties through the choice of captured atoms.
The increasing worldwide energy consumption calls for the design of more efficient energy systems. Thermoelectrics could be used to convert waste heat back to useful electric energy if only more efficient materials were available. The ideal thermoelectric material combines high electrical conductivity and thermopower with low thermal conductivity. In this regard, the intermetallic type-I clathrates show promise with their exceedingly low lattice thermal conductivities [1]. Here we report the successful incorporation of cerium as guest atom into the clathrate crystal structure. In many simpler intermetallic compounds, this rare earth element is known to lead, via the Kondo interaction, to strong correlation phenomena including the ocurrence of giant thermopowers at low temperatures [2]. Indeed, we observe a 50% enhancement of the thermopower compared to a rare earth-free reference material. Importantly, this enhancement occurs at high temperatures and we suggest that a `rattling enhanced Kondo interaction [3] underlies this effect.
The object of this study is the kinetic process of solid-liquid first-order phase transition - melting of carbon dioxide CS-I hydrate with various cavity occupation ratios. The work was done within a framework of study on the local structure of water molecules. These include the time depending change of the short-range order at temperatures close to the melting point and comparison with hexagonal ice structure. Using molecular dynamics method, dependencies of the internal energy of the studied systems on the time of heating were found. Jumps in the internal energy of solids in the range at 275-300 K indicate a phase transition. The study of oxygen-oxygen radial distribution and hydrogen-oxygen-oxygen mutual orientation angles between molecules detached at no more than 3.2 angstroms allowed to find the H-bond coordination number of all molecules and full number of H-bonds and showed the instant (less than 1 nanosecond) reorganization of short-range order of all molecules. The structure analysis of every neighbor water molecules pairs showed the ~10-15 percents decrease of H-bond number after the melting whereas all molecules form single long-range hydrogen bond network. The analysis of hydrogen bond network showed the minor changes in the H-bond interaction energy at solid-liquid phase transition.
A ternary type-I Si clathrate, K8AlxSi46-x, which is a candidate functional material composed of abundant non-toxic elements, was synthesized and its transport properties were investigated at temperatures ranging from 10 to 320 K. The synthesized compound is confirmed to be the ternary type-I Si clathrate K8Al7Si39 with a lattice parameter of a = 10.442 A using neutron powder diffractometry and inductively coupled plasma optical emission spectrometry. Electrical resistivity and Hall coefficient measurements revealed that K8Al7Si39 is a metal with electrons as the dominant carriers at a density of approximately 1x10^27 /m3. The value of Seebeck coefficient for K8Al7Si39 is negative and its absolute value increases with the temperature. The temperature dependence of the thermal conductivity is similar to that for a crystalline solid. The dimensionless figure of merit is approximately 0.01 at 300 K, which is comparable to that for other ternary Si clathrates.
Cerium oxide (ceria, CeO2) is one of the most promising mixed ionic and electronic conducting materials. Previous atomistic analysis has covered widely the effects of substitution on oxygen vacancy migration. However, an in-depth analysis of the role of cation substitution beyond trivalent cations has rarely been explored. Here, we investigate soluble monovalent, divalent, trivalent and tetravalent cation substituents. By combining classical simulations and quantum mechanical calculations, we provide an insight into defect association energies between substituent cations and oxygen vacancies as well as their effects on the diffusion mechanisms. Our simulations indicate that oxygen ionic diffusivity of subvalent cation-substituted systems follows the order Gd>Ca>Na. With the same charge, a larger size mismatch with Ce cation yields a lower oxygen ionic diffusivity, i.e., Na>K, Ca>Ni, Gd>Al. Based on these trends, we identify species that could tune the oxygen ionic diffusivity: we estimate that the optimum oxygen vacancy concentration for achieving fast oxygen ionic transport is 2.5% for GdxCe1-xO2-x/2, CaxCe1-xO2-x and NaxCe1-xO2-3x/2 at 800 K. Remarkably, such a concentration is not constant and shifts gradually to higher values as the temperature is increased. We find that co-substitutions can enhance the impact of the single substitutions beyond that expected by their simple addition. Furthermore, we identify preferential oxygen ion migration pathways, which illustrate the electro-steric effects of substituent cations in determining the energy barrier of oxygen ion migration. Such fundamental insights into the factors that govern the oxygen diffusion coefficient and migration energy would enable design criteria to be defined for tuning the ionic properties of the material, e.g., by co-doping.
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