High-Pressure Synthesis of Magnetic Neodymium Polyhydrides

TL;DR

This study reports the synthesis of new neodymium hydrides under high pressure, explores their magnetic and superconducting properties, and predicts potential high-temperature superconductivity in these materials.

Contribution

It introduces several novel neodymium hydrides synthesized at high pressures and provides insights into their magnetic order and potential superconducting behavior.

Findings

Discovery of new Nd-H phases at high pressures.

Possible superconductivity at ~4.5 K in NdH9.

Predicted high Néel temperatures for some hydrides.

Abstract

The current search for room-temperature superconductivity is inspired by the unique properties of the electron-phonon interaction in metal superhydrides. Encouraged by the recently found highest-$T_C$ superconductor fcc-$LaH_{10}$, here we discover several superhydrides of another lanthanide - neodymium. We identify three novel metallic Nd-H phases at pressure range from 85 to 135 GPa: $I4/mmm$-$NdH_4$, $C2/c$-$NdH_7$, $P6_3/mmc$-$NdH_9$, synthesized by laser-heating metal samples in NH3BH3 media for in situ generation of hydrogen. A lower trihydride $Fm\bar{3}m$-$NdH_3$ is found at pressures from 2 to 52 GPa. $I4/mmm$-$NdH_4$ and $C2/c$-$NdH_7$ are stable from 135 down to 85 GPa, and $P6_3/mmc$-$NdH_9$ from 110 to 130 GPa. Measurements of the electrical resistance of NdH9 demonstrate a possible superconducting transition at ~4.5 K in $P6_3/mmc$-$NdH_9$. Our theoretical calculations predict that all the neodymium hydrides have antiferromagnetic order at pressures below 150 GPa and represent one of the first discovered examples of strongly correlated superhydrides with large exchange spin-splitting in the electron band structure (> 450 meV). The critical N$\'e$el temperatures for new neodymium hydrides are estimated using the mean-field approximation as about 4 K ($NdH_4$), 251 K ($NdH_7$) and 136 K ($NdH_9$).