Superhydrides have complex hydrogenic sublattices and are important prototypes for studying metallic hydrogen and high-temperature superconductors. Encouraged by the results on LaH10, in consideration of the differences between La and Pr, Pr-H system is especially worth studying because of the magnetism and valence-band f-electrons in element Pr. Here we successfully synthesized praseodymium superhydrides (PrH9) in laser-heated diamond anvil cells. Synchrotron X-ray diffraction (XRD) analysis demonstrated the presence of previously predicted F4 ̅ 3m-PrH9 and unexpected P63/mmc-PrH9 phases. Moreover, Fm3 ̅ m-PrH3, P4/nmm-PrH3-δ and Fm3 ̅ m-PrH1+x were found below 52 GPa. F4 ̅ 3m-PrH9 and P63/mmc-PrH9 were stable above 100 GPa in experiment. Experimental studies of electrical resistance in the PrH9 sample showed the emergence of superconducting transition (Tc) below 9 K and a dependent Tc on applied magnetic field. Theoretical calculations indicate that magnetic order and electron-phonon interaction coexist in a very close range of pressures in the PrH9 sample which may contribute to its low superconducting temperature Tc. Our results highlight the intimate connections among hydrogenic sublattices, density of states, magnetism and superconductivity in Pr-based superhydrides.

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Following the discovery of high-temperature superconductivity in the La–H system, we studied the formation of new chemical compounds in the barium-hydrogen system at pressures from 75 to 173 GPa. Using in situ generation of hydrogen from NH3BH3, we synthesized previously unknown superhydride BaH12 with a pseudocubic (fcc) Ba sublattice in four independent experiments. Density functional theory calculations indicate close agreement between the theoretical and experimental equations of state. In addition, we identified previously known P6/mmm-BaH2 and possibly BaH10 and BaH6 as impurities in the samples. Ab initio calculations show that newly discovered semimetallic BaH12 contains H2 and H3– molecular units and detached H12 chains which are formed as a result of a Peierls-type distortion of the cubic cage structure. Barium dodecahydride is a unique molecular hydride with metallic conductivity that demonstrates the superconducting transition around 20 K at 140 GPa.

We conducted a joint experimental−theoretical investigation of the high-pressure chemistry of europium polyhydrides at pressures of 86−130 GPa. We discovered several novel magnetic Eu superhydrides stabilized by anharmonic effects: cubic EuH 9 , hexagonal EuH 9 , and an unexpected cubic (Pm3n) clathrate phase, Eu 8 H 46 . Monte Carlo simulations indicate that cubic EuH 9 has antiferromagnetic ordering with T N of up to 24 K, whereas hexagonal EuH 9 and Pm3n-Eu 8 H 46 possess ferromagnetic ordering with T C = 137 and 336 K, respectively. The electron−phonon interaction is weak in all studied europium hydrides, and their magnetic ordering excludes s-wave superconductivity, except, perhaps, for distorted pseudohexagonal EuH 9 . The equations of state predicted within the DFT+U approach (U − J were found within linear response theory) are in close agreement with the experimental data. This work shows the great influence of the atomic radius on symmetry-breaking distortions of the crystal structures of superhydrides and on their thermodynamic stability.

Hybrid organic–inorganic perovskites (HOIPs) have gained substantial attention due to their excellent photovoltaic and optoelectronic properties.