Template induced precursor formation in heterogeneous nucleation -- Controlling polymorph selection and nucleation efficiency

Abstract

We present an atomistic study of heterogeneous nucleation in Ni employing transition path sampling, which reveals a template precursor-mediated mechanism of crystallization. Most notably, we find that the ability of tiny templates to modify the structural features of the liquid and promote the formation of precursor regions with enhanced bond-orientational order is key to determine their nucleation efficiency and the polymorphs that crystallize. Our results reveal an intrinsic link between liquid heterogeneity and the nucleating ability of templates, which significantly advances our understanding towards the control of nucleation efficiency and polymorph selection.