Time-Resolved Study of Crystallization in Deeply Cooled Liquid Parahydrogen

Abstract

We present real-time measurements of the crystallization process occurring in liquid para-hydrogen (para-H(2)) quenched to ≈0.65T(m) (T(m)=13.8 K is the melting point of bulk liquid para-H(2)). The combination of high spatial resolution Raman spectroscopy and liquid microjet generation allows, in situ, capturing structural changes with ∼10(-8) s time resolution. Our results provide a crystal growth rate that rules out a thermally activated freezing process and reveal that the quenched melt freezes into a metastable polymorph, which undergoes a structural transition. The achieved temporal control offers new opportunities for exploring the elementary processes of nonequilibrium phase transformations in supercooled liquids.