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Area of Science:

  • Condensed Matter Physics
  • Materials Science
  • Quantum Mechanics

Background:

  • High-pressure lanthanum polyhydrides exhibit superconductivity near room temperature.
  • Previous studies often simplified nonstoichiometric LaH10±δ to LaH10, neglecting defects.
  • The positive pressure dependence of critical temperature (Tc) below 150 GPa remained unexplained.

Purpose of the Study:

  • To investigate nuclear quantum effects (NQE) in nonstoichiometric lanthanum polyhydride.
  • To explain the observed superconductivity and pressure dependence of Tc.
  • To understand the role of stoichiometric defects and proton diffusion.

Main Methods:

  • Theoretical investigation of nuclear quantum effects.
  • Analysis of X-ray diffraction (XRD) data for LaH9.63.
  • Modeling of proton diffusion and its impact on electronic structure and electron-phonon coupling.

Main Results:

  • Significant NQE observed, leading to quantum proton diffusion in LaH9.63 at 150 GPa and 240 K.
  • Diffusion coefficient reached ~10-7 cm2/s, near the upper bound for interstitial hydrides.
  • Explained the positive pressure dependence of Tc by modulation of electronic structure and electron-phonon coupling due to lattice distortions.

Conclusions:

  • Quantum proton fluxion coexists with hydrogen-induced superconductivity in lanthanum polyhydrides.
  • Stoichiometric defects are crucial for understanding the quantum fluxional nature and superconductivity.
  • Provides insight into the behavior of nonstoichiometric hydrogen-rich materials under high pressure.