Melting Domain Size and Recrystallization Dynamics of Ice Revealed by Time-Resolved X-ray Scattering

TL;DR

This study uses time-resolved x-ray scattering to investigate the ultrafast melting and recrystallization of ice, revealing domain size dynamics and superheating phenomena at nanosecond to microsecond timescales.

Contribution

It provides direct structural insights into ice melting and recrystallization dynamics using combined WAXS and SAXS techniques with ultrafast laser heating.

Findings

Partial melting of ~13% occurs at around 20 ns.

Liquid domain size grows from 2.5 nm to 4.5 nm within 100 ns.

Recrystallization reduces liquid domain size on microsecond timescales.

Abstract

The phase transition between water and ice is ubiquitous and one of the most important phenomena in nature. Here, we performed time-resolved x-ray scattering experiments capturing the melting and recrystallization dynamics of ice. The ultrafast heating of ice I is induced by an IR laser pulse and probed with an intense x-ray pulse, which provided us with direct structural information on different length scales. From the wide-angle x-ray scattering (WAXS) patterns, the molten fraction, as well as the corresponding temperature at each delay, were determined. The small-angle x-ray scattering (SAXS) patterns, together with the information extracted from the WAXS analysis, provided the time-dependent change of the size and the number of the liquid domains. The results show partial melting (~13 %) and superheating of ice occurring at around 20 ns. After 100 ns, the average size of the liquid domains grows from about 2.5 nm to 4.5 nm by the coalescence of approximately six adjacent domains. Subsequently, we capture the recrystallization of the liquid domains, which occurs on microsecond timescales due to the cooling by heat dissipation and results to a decrease of the average liquid domain size.