Theoretical investigation of high-pressure phase stability and potential superconductivity of Ce–S–H ternary hydrides

Abstract

The discovery of high-temperature superconductivity in lanthanide- and sulfur-hydrides has attracted substantial interest recently. Here, we systematically investigate the high-pressure phase stability and superconducting properties of Ce–S–H ternary hydrides using first-principles calculations coupled with swarm-intelligence-based structure prediction methods. Our calculations reveal that all considered compositions (CeSH₂, CeSH₃, CeSH₆, CeSH₈, CeSH₉ and CeSH₁₀) exhibit thermodynamic and dynamic stability within the pressure range of 50–300 GPa. The hydrogen configurations in these compounds feature diverse motifs, including isolated H atoms, molecular “H₂” and “H₃” units, and H–S covalent networks, as validated by electron localization function (ELF) and Bader charge analysis. Notably, electron–phonon coupling (EPC) calculations identify Cm-CeSH₉ and Cc-CeSH₁₀ as promising superconductors, with transition temperatures (T_c) of 73.3 K at 150 GPa and 95.7 K at 300 GPa, respectively. These findings highlight the potential of Ce–S–H systems as high-T_c candidates under high-pressure conditions.