Link to Densify: Topological Transitions and Origin of Hysteresis During the (De)Compression of Amorphous Ices

TL;DR

This study reveals a topological transition in hydrogen bond networks during the phase change between low-density and high-density amorphous ices, explaining hysteresis and mechanical fragility.

Contribution

It uncovers a topological transition in hydrogen bond networks that explains the hysteresis cycle in amorphous ice phase transitions.

Findings

Topological differences in hydrogen bond networks between LDA and HDA.

Transient topological motifs lead to mechanical fragility.

Topological transition may be a generic densification mechanism.

Abstract

In this Letter we study the phase transition between amorphous ices and the nature of the hysteresis cycle separating them. We discover that a topological transition takes place as the system transforms from low-density amorphous ice (LDA) at low pressures, to high-density amorphous ice (HDA) at high pressures. Specifically, we uncover that the hydrogen bond network (HBN) displays qualitatively different topologies in the LDA and HDA phases: the former characterised by disentangled loop motifs, while the latter displaying topologically complex and metastable Hopf-linked and knotted configurations. At the phase transition, the transient opening of the HBN topological motifs yields mechanical fragility on the macroscale. Our results provide a detailed microscopic description of the topological nature of the phase transition and the hysteresis cycle between amorphous ices. We argue that the topological transition discovered in this work may not only improve our understanding of amorphous ices but represent a generic mechanism for the densification of network-forming materials.