Synthesis of Mg${}_2$IrH${}_5$: A potential pathway to high-$T_c$ hydride superconductivity at ambient pressure

Abstract

Following long-standing predictions associated with hydrogen, high-temperature superconductivity has recently been observed in several hydride-based materials. Nevertheless, these high-$T_c$ phases only exist at extremely high pressures, and achieving high transition temperatures at ambient pressure remains a major challenge. Recent predictions of the complex hydride Mg${}_2$IrH${}_6$ may help overcome this challenge with calculations of high-$T_c$ superconductivity (65 K$<T_c<$ 170 K) in a material that is stable at atmospheric pressure. In this work, the synthesis of Mg${}_2$IrH${}_6$ was targeted over a broad range of $P$-$T$ conditions, and the resulting products were characterized using X-ray diffraction (XRD) and vibrational spectroscopy, in concert with first-principles calculations. The results indicate that the charge-balanced complex hydride Mg${}_2$IrH${}_5$ is more stable over all conditions tested up to ca 28 GPa. The resulting hydride is isostructural with the predicted superconducting Mg${}_2$IrH${}_6$ phase except for a single hydrogen vacancy, which shows a favorable replacement barrier upon insertion of hydrogen into the lattice. Bulk Mg${}_2$IrH${}_5$ is readily accessible at mild $P$-$T$ conditions and may thus represent a convenient platform to access superconducting Mg${}_2$IrH${}_6$ via non-equilibrium processing methods.

18 pages, 17 Figures