Uranium polyhydrides at moderate pressures: prediction, synthesis, and expected superconductivity

TL;DR

This study predicts and experimentally confirms the existence of numerous uranium hydrides at moderate pressures, many of which are expected to be high-temperature superconductors, expanding the understanding of hydrogen-rich materials.

Contribution

The paper introduces 14 new uranium hydrides predicted via ab initio methods and confirms several phases experimentally, highlighting their potential as high-temperature superconductors.

Findings

Confirmed UH7, UH8, and UH5 phases experimentally.

Predicted UH7 to be a high-Tc superconductor with 44-66 K.

Discovered a rich chemistry of uranium hydrides with unusual H8 clusters.

Abstract

Hydrogen-rich hydrides attract great attention due to recent theoretical (1) and then experimental discovery of record high-temperature superconductivity in H3S (Tc = 203 K at 155 GPa (2)). Here we search for stable uranium hydrides at pressures up to 500 GPa using ab initio evolutionary crystal structure prediction. Chemistry of the U-H system turned out to be extremely rich, with 14 new compounds, including hydrogen-rich UH5, UH6, U2H13, UH7, UH8, U2H17, and UH9. Their crystal structures are based on either common f.c.c. or h.c.p. uranium sublattice and unusual H8 cubic clusters. Our high-pressure experiments at 1-103 GPa confirm the predicted UH7, UH8, and three different phases of UH5, raising confidence about predictions of the other phases. Many of the newly predicted phases are expected to be high-temperature superconductors. The highest-Tc superconductor is UH7 predicted to be thermodynamically stable at pressures above 22 GPa (with Tc = 44-54 K) and this phase remains dynamically stable upon decompression to zero pressure (with Tc = 57-66 K).