The high pressure structures, metallization, and superconductivity of recently synthesized H2-containing compounds (H2S)2H2 are elucidated by ab initio calculations. The ordered crystal structure with P1 symmetry is determined, supported by the good agreement between theoretical and experimental X-ray diffraction data, equation of states, and Raman spectra. The Cccm structure is favorable with partial hydrogen bond symmetrization above 37 GPa. Upon further compression, H2 molecules disappear and two intriguing metallic structures with R3m and Im-3m symmetries are reconstructive above 111 and 180 GPa, respectively. The predicted metallization pressure is 111 GPa, which is approximately one-third of the currently suggested metallization pressure of bulk molecular hydrogen. Application of the Allen-Dynes-modified McMillan equation for the Im-3m structure yields high Tc values of 191 K to 204 K at 200 GPa, which is among the highest values reported for H2-rich van der Waals compounds and MH3 type hydride thus far.
The structures and properties of rhenium nitrides are studied with density function based first principle method. New candidate ground states or high-pressure phases at Re:N ratios of 3:2, 1:3, and 1:4 are identified via a series of evolutionary structure searches. We find that the 3D polyhedral stacking with strong covalent N-N and Re-N bonding could stabilize Re nitrides to form nitrogen rich phases, meanwhile, remarkably improve the mechanical performance than that of sub-nitrides, as Re3N, Re2N, and Re3N2. By evaluating the trends of the crystal configuration, electronic structure, elastic properties, and hardness as a function of the N concentration, we proves that the N content is the key factor affecting the metallicity and hardness of Re nitrides.
Niobium-nitrogen compounds, which are potential candidates for superhard multifunctional materials, may possess multiple stoichiometries and structures under pressure. Based on ab initio evolutionary structural searches, we predict three ground states (oP6-Nb2N, CW-NbN, and hP22-Nb5N6) and six stable high pressure phases (ε-NbN, AsNi-NbN, U2S3-Nb2N3, oC24-NbN2, mP8-NbN3, and mP20-NbN4) for Nb-N compounds at pressures up to 100 GPa. Among them, the oP6-Nb2N, oC24-NbN2, mP8-NbN3, and mP20-NbN4 have never been reported, and N-rich oC24-NbN2, mP8-NbN3, and mP20-NbN4 high pressure phases are recoverable to ambient pressure. We find that the structure of N-rich Nb-N compounds consists of NbNx polyhedral stacking configurations and connected with Nn (n = 2, 3, 4, and n) polymerizations, which can remarkably improve the elastic modulus. It is found that CW-NbN and mP20-NbN4 are two potential ultra-incompressible and hard materials with the hardness calculated to be 24.56 and 19.86 GPa, respectively, while other N-rich phases such as U2S3-Nb2N3, oC24-NbN2, and mP8-NbN3 are soft materials. Detailed electronic structure and chemical bonding analysis proved that the high hardness of CW-NbN and mP20-NbN4 stems from the strong covalent bonding and the fullfilled Nb-N bonding and antibonding states.
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