Pre-critical fluctuations and what they disclose about heterogeneous crystal nucleation - Archive ouverte HAL
Journal Articles Nature Communications Year : 2017

Pre-critical fluctuations and what they disclose about heterogeneous crystal nucleation

Abstract

Heterogeneous crystal nucleation is ubiquitous in nature and at the heart of many industrial applications. At the molecular scale, however, major gaps in understanding this phenomenon persist. Here we investigate through molecular dynamics simulations how the formation of precritical crystalline clusters is connected to the kinetics of nucleation. Considering heterogeneous water freezing as a prototypical scenario of practical relevance, we find that precritical fluctuations connote which crystalline polymorph will form. The emergence of metastable phases can thus be promoted by templating crystal faces characteristic of specific polymorphs. As a consequence, heterogeneous classical nucleation theory cannot describe our simulation results, because the different substrates lead to the formation of different ice polytypes. We discuss how the issue of polymorphism needs to be incorporated into analysis and comparison of heterogeneous and homogeneous nucleation. Our results will help to interpret and analyze the growing number of experiments and simulations dealing with crystal polymorph selection.
Fichier principal
Vignette du fichier
s41467-017-02300-x.pdf (1.31 Mo) Télécharger le fichier
Origin Publication funded by an institution
Loading...

Dates and versions

hal-01678826 , version 1 (09-01-2018)

Licence

Identifiers

Cite

Martin Fitzner, Gabriele C Sosso, Fabio Pietrucci, Silvio Pipolo, Angelos Michaelides. Pre-critical fluctuations and what they disclose about heterogeneous crystal nucleation. Nature Communications, 2017, 8, pp.2257. ⟨10.1038/s41467-017-02300-x⟩. ⟨hal-01678826⟩
696 View
117 Download

Altmetric

Share

More