High-pressure synthesis of seven lanthanum hydrides with a significant variability of hydrogen content

The lanthanum-hydrogen system has attracted significant attention following the report of superconductivity in LaH10 at near-ambient temperatures and high pressures. Phases other than LaH10 are suspected to be synthesized based on both powder X-ray diffraction and resistivity data, although they have not yet been identified. Here, we present the results of our single-crystal X-ray diffraction studies on this system, supported by density functional theory calculations, which reveal an unexpected chemical and structural diversity of lanthanum hydrides synthesized in the range of 50 to 180 GPa. Seven lanthanum hydrides were produced, LaH3, LaH~4, LaH4+δ, La4H23, LaH6+δ, LaH9+δ, and LaH10+δ, and the atomic coordinates of lanthanum in their structures determined. The regularities in rare-earth element hydrides unveiled here provide clues to guide the search for other synthesizable hydrides and candidate high-temperature superconductors. The hydrogen content variability in lanthanum hydrides and the samples’ phase heterogeneity underline the challenges related to assessing potentially superconducting phases and the nature of electronic transitions in high-pressure hydrides.Funding: Alexander von Humboldt Foundation; Deutsche Forschungsgemeinschaft (DFG) [LA-4916/1-1, DU 954-11/1, DU 393-9/2, DU 393-13/1, DFG FOR2125, WI1232]; UKRI Future Leaders Fellowship [MR/V025724/1]; Federal Ministry of Education and Research, Germany (BMBF) [05K19WC1]; BIOVIA through the Science Ambassador program; Swedish Government Strategic Research Area inMaterials Science on Functional Materials at Linkoping University (Faculty Grant SFO-Mat-LiU) [2009 00971]; Knut and Alice Wallenberg Foundation [KAW-2018.0194]; Swedish e-science Research Center (SeRC); Swedish Research Council (VR) grant [2019-05600]; Swedish Research Council (VR) program [2020-04630]; Swedish e-Science ResearchCentre (SeRC)