High-pressure phase stability and superconductivity in La-Zr-H hydrides
Hydrogen-rich ternary hydrides are promising candidates for high-Tc superconductivity at megabar pressures, yet their chemical space is vast and largely unexplored. Combining evolutionary structure searches with first-principles calculations, we comprehensively investigate the La-Zr-H ternary system in the 150-300 GPa pressure range. Zero-point energy-corrected convex hull analysis identifies multiple stable superconducting phases, including R3m-Zr2H17 at 300 GPa and P6/mmm-LaZr2H24 at 200 GPa, both of which are thermodynamically and dynamically stable and exhibit strong electron-phonon coupling. Solution of the Eliashberg equations predicts high superconducting transition temperatures of Tc = 209 K for R3m-Zr2H17 at 300 GPa and Tc = 202 K for P6/mmm-LaZr2H24 at 200 GPa. In addition to these stable phases, we identify a high-symmetry metastable compound, P6m2-LaZrH18, which lies just 0.027 eV/atom above the convex hull yet remains dynamically stable and exhibits a high predicted Tc of 206 K at 300 GPa. We find that, across all phases, the elevated Tc correlates with the high-symmetry structure with dense hydrogen cages, favorable electron counts per hydrogen, and a large hydrogen-derived density of states at the Fermi level. Finally, a random- forest machine learning model, trained on diverse hydrides superconductivity data, reproduces these structure-property trends across predicted structures, enabling to identify potential hydrides with high predicted Tc for targeted follow-up calculations and future high-pressure experiments.