Ab initio investigation on structural stability and phonon-mediated superconductivity in 2D-hydrogenated M2X (M= Mo, V, Zr; X=C, N) MXene monolayer

Abstract

We present a comprehensive first-principles study of hydrogenated M2X (M = Mo, V, Zr; X = C, N) MXene monolayers, focusing on their structural stability, electronic properties, and superconducting behavior. Structural optimizations combined with phonon spectra reveal that partial hydrogenation (1H and 2H) is dynamically stable across most compositions, while full hydrogenation (4H) generally induces lattice instabilities. A notable exception is Zr2CH4, which retains dynamical stability even under maximum hydrogen coverage. Electronic structure analysis shows that all hydrogenated MXenes remain metallic, with the Fermi level dominated by transition-metal d orbitals. In Zr2CH4, a Dirac-like band crossing at the Fermi level is observed, which is gapped by spin-orbit coupling (SOC), yielding a finite gap of 0.095 eV. Electron-phonon coupling (EPC) calculations demonstrate that Mo-based MXenes exhibit strong EPC, with coupling constants lambda = 0.95 (Mo2CH), 1.23 (Mo2NH), and 1.55 (Mo2NH2), corresponding to superconducting critical temperatures Tc about 15 to 22 K within the Allen-Dynes framework (mu* = 0.10). By contrast, V- and Zr-based MXenes display weak EPC and negligible Tc, with Zr2CH4 being a special case hosting Dirac-like states rather than superconductivity. Our findings highlight hydrogen functionalization as an effective strategy to stabilize MXene monolayers and to tune their low-energy physics, revealing Mo-based nitride MXenes as promising phonon-mediated superconductors, while Zr2CH4 emerges as a candidate for Dirac physics.