Transformation of hexagonal Lu to cubic LuH2+x_{2+x} single-crystalline films

With the recent report of near ambient superconductivity at room temperature in the N-doped lutetium hydride (Lu-H-N) system, the understanding of cubic Lu-H compounds has attracted worldwide attention. Generally, compared to polycrystal structures with non-negligible impurities, the single-crystalline form of materials with high purity can provide an opportunity to show their hidden properties. However, the experimental synthesis of single-crystalline cubic Lu-H compounds has not been reported thus far. Here, we developed an easy way to synthesize highly pure LuH$_{2+x}$ single-crystalline films by the post-annealing of Lu single-crystalline films (purity of 99.99%) in the H$_2$ atmosphere. The crystal and electronic structures of films were characterized by X-ray diffraction, Raman spectroscopy, and electrical transport. Interestingly, Lu films are silver-white and metallic, whereas their transformed LuH$_{2+x}$ films become purple-red and insulating, indicating the formation of an unreported electronic state of Lu-H compounds possibly. Our work provides a novel route to synthesize and explore more single-crystalline Lu-H compounds

Lu-H-N phase diagram from first-principles calculations

Using a comprehensive structure search and high-throughput first-principles calculations of 1483 compounds, this study presents the phase diagram of Lu-H-N. The formation energy landscape of Lu-H-N was derived and utilized to assess the thermodynamic stability of compounds. Results indicate that there are no stable Lu-H-N ternary structures in this system, but metastable ternary structures, such as Lu20H2N17 (C2/m), Lu2H2N (P3-m1), were observed with small Ehull (< 100 meV/atom). Moreover, applying hydrostatic pressure up to 10 GPa causes the energy convex hull of the Lu-H-N to shift its shape and stabilizes binary phases such as LuN9 and Lu10H21. Additionally, interstitial empty sites in LuH2 were noted, which may explain the formation of Lu10H21 and LuH3-xNy. To provide a basis for comparison, X-ray diffraction patterns and electronic structures of some compounds are also presented