Designing multicomponent hydrides with potential high T c superconductivity

Denchfield, Adam; Park, Hyowon; Hemley, Russell J

doi:10.1073/pnas.2413096121

While hydrogen-rich materials have been demonstrated to exhibit high T_csuperconductivity at high pressures, there is an ongoing search for ternary, quaternary, and more chemically complex hydrides that achieve such high critical temperatures at much lower pressures. First-principles searches are impeded by the computational complexity of solving the Eliashberg equations for large, complex crystal structures. Here, we adopt a simplified approach using electronic indicators previously established to be correlated with superconductivity in hydrides. This is used to study complex hydride structures, which are predicted to exhibit promisingly high critical temperatures for superconductivity. In particular, we propose three classes of hydrides inspired by the Fm

\bar{3}

m RH

_{3}

structures that exhibit strong hydrogen network connectivity, as defined through the electron localization function. The first class [RH

_{11}

X

_{3}

Y] is based on a Pm

\bar{3}

m structure showing moderately high T_c, where the T_cestimate from electronic properties is compared with direct Eliashberg calculations and found to be surprisingly accurate. The second class of structures [(RH

_{11}

)

_{2}

X

_{6}

YZ] improves on this with promisingly high density of states with dominant hydrogen character at the Fermi energy, typically enhancing T_c. The third class [(R

^{1}

H

_{11}

)(R

^{2}

H

_{11}

)X

_{6}

YZ] improves the strong hydrogen network connectivity by introducing anisotropy in the hydrogen network through a specific doping pattern. These design principles and associated model structures provide flexibility to optimize both T_cand the structural stability of complex hydrides.

More Like this