Interface-dependent Phase Transitions and Ultrafast Hydrogen Superionic Diffusion of H2O Ice

TL;DR

This study uses advanced simulations to show how interfaces in high-pressure ice samples significantly influence phase transitions and superionic behavior, revealing new stable phases and explaining experimental discrepancies.

Contribution

It demonstrates the impact of interfaces on high-pressure ice properties using neural network-enhanced molecular dynamics, uncovering new phase stability fields and transition mechanisms.

Findings

Interface lowers hydrogen superionic transition temperature.

Spontaneous bcc to fcc ice transition via inverse Bain mechanism.

Predicted fcc ice at much lower pressures than previously thought.

Abstract

High-pressure experiments using diamond anvils have revealed novel properties and phase behavior of H2O under extreme conditions. When contained in diamond-anvil cells, the H2O samples are usually in direct contact with the diamond anvil. However, the extent to which this interface affects measured pressure-induced properties and behavior, including coexistence lines of ice phases, remains unknown. Combining artificial neural network methods and active learning schemes with large-scale molecular dynamics simulations, we elucidate the interfacial effects on various properties of high-pressure ice phases, including superionic states, solid-solid phase transitions, and melting. The results reveal that the presence of this interface can significantly lower the hydrogen superionic transition temperature. Remarkably, the interface can also induce a spontaneous transition from bcc- to fcc-based ice following the inverse Bain mechanism. Further, we redefined a stability field of bcc and fcc ice below the melting line and predicted the existence of fcc ice at much lower pressures than previously thought. More broadly, the results emphasize the importance of interface effects in understanding a wide range of phenomena reported in experimental studies of ice under pressure, including inconsistencies between theoretical and experimental results of this fundamental system.