The Critical Metallization of Hydrogen in Pressurized LaBeH8 Hydride

TL;DR

This paper develops a theoretical framework combining molecular dynamics and electronic structure analysis to understand hydrogen metallization in hydrides, exemplified by LaBeH8, revealing critical behaviors during phase transitions relevant to superconductivity.

Contribution

It introduces a novel theoretical framework to quantify hydrogen atomization and metallization in hydrides, addressing a key gap in understanding phase transition mechanisms.

Findings

Identification of three hydrogen orderings: molecular, sublattice, and warm hydrogens.

Discovery of critical metallization behaviors including superionicity and metallicity.

Insights into synthesis routes for metastable phases of superconducting hydrides.

Abstract

Behaviours of hydrogen, such as fluidity and metallicity, are crucial for our understanding of planetary interiors and the emerging field of high-temperature superconducting hydrides. These behaviours were discovered in complex phase diagrams of hydrogen and hydrides, however, the transition mechanism of behaviours driven by temperature, pressure and chemical compression remain unclear, particularly in the processes of metallization. Until now, a comprehensive theoretical framework to quantify atomization and metallization of hydrogen in phase diagram of hydrides has been lacking. In this study, we address this gap by combining molecular dynamics and electronic structure analysis to propose a theoretical framework, which clarify the content and properties of atomic hydrogen under various temperature and pressure conditions and chemical compression exerted by non-hydrogen elements in hydrides. Applying this framework to the superconducting hydride LaBeH8, we identify three general hydrogen orderings within its phase diagram: molecular, sublattice and warm hydrogens. During the phase transition from molecule to sublattice, hydrogen exhibits different properties from three general hydrogen orderings, such as fast superionicity, metallicity and unusual atomic content response to temperature. These abnormal behaviours were defined as the critical metallization of hydrogen, which not only suggests a potential synthesis route for the metastable phase but also provides valuable insights into the complex synthetic products of superconducting hydrides.