Tuning Chemical Precompression: Theoretical Design and Crystal Chemistry of Novel Hydrides in the Quest for Warm and Light Superconductivity at Ambient Pressures

Abstract

Over the past decade, a combination of crystal structure prediction techniques and experimental synthetic work has thoroughly explored the phase diagrams of binary hydrides under pressure. The fruitfulness of this dual approach is demonstrated in the recent identification of several superconducting hydrides with \(T_c\)s approaching room temperature. We start with an overview of the computational procedures for predicting stable structures and estimating their propensity for superconductivity. A survey of phases with high \(T_c\) reveals some common structural features that appear conducive to the strong coupling of the electronic structure with atomic vibrations that leads to superconductivity. We discuss the stability and superconducting properties of phases containing two of these -- molecular H\(_2\) units mixed with atomic H and hydrogenic clathrate-like cages -- as well as more unique motifs. Finally, we argue that ternary hydride phases, which are far less-explored, are a promising route to achieving simultaneously superconductivity at high temperatures and stability at low pressures. Several ternary hydrides arise from the addition of a third element to a known binary hydride structure through site mixing or onto a new site -- and several more are based on altogether new structural motifs.