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Impact of ionic quantum fluctuations on the thermodynamic stability and superconductivity of LaBH₈

Abstract

The recent prediction of a metastable high-symmetry Fm3m phase of LaBH₈ gives hopes to reach high superconducting critical temperatures at affordable pressures among ternary hydrogen-rich compounds. Making use of first-principles calculations within density functional theory and the stochastic self-consistent harmonic approximation, we determine that ionic quantum fluctuations drive the system dynamically unstable below 77 GPa, a much higher pressure than the 45 GPa expected classically. Quantum anharmonic effects stretch the covalent B-H bond in the BH₈ units of the structure and, consequently, soften all hydrogen-character modes. Above 77 GPa Fm3m LaBH₈ remains metastable and, interestingly, its superconducting critical temperature is largely enhanced by quantum anharmonic effects, reaching critical temperatures around 170 K at the verge of the dynamical instability. Our results suggest that low pressure metastable phases with covalently bonded symmetric XH₈ units will be destabilized by ionic quantum fluctuations.

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