A Comprehensive Study on A 2 PdH 2 : From Ambient to High Pressure

Abstract

We present a comprehensive first-principles study of the structural stability and superconducting behavior of Li2PdH2 under high pressure. Using random structure searching and phonon calculations, we identify a pressure-induced phase transition from a tetragonal I4/mmm structure, stable up to ≈ 5 GPa, to a monoclinic C2/m phase that remains thermodynamically stable up to 50 GPa. Superconductivity is absent in the tetragonal phase, even when anharmonic effects are considered, due to weak electron-phonon coupling and limited hydrogen involvement near the Fermi level. In contrast, the monoclinic phase exhibits a weak but pressure-enhanced superconducting transition, with Tc increasing from 0.6 K at 10 GPa to 4.7 K at 50 GPa, mainly driven by low-frequency Liand Pd-derived phonon modes. We further explore the isostructural A2PdH2 (A = Na, K, Rb, Cs) series to evaluate the impact of alkali-metal substitution on stability and superconductivity. Na, K, and Rb analogs retain dynamic stability at ambient pressure, with weak superconducting critical temperatures of 3.2 K, 2.1 K, and negligible Tc, respectively. Cs2PdH2, however, exhibits phonon instabilities, suggesting a need for external stabilization. These findings highlight the delicate balance between lattice dynamics, electronic structure, and atomic mass in tuning superconductivity in palladium-based hydrides.