Template-Induced Precursor Formation in Heterogeneous Nucleation: Controlling Polymorph Selection and Nucleation Efficiency

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 determining their nucleation efficiency and the polymorphs that crystallize. Our results reveal an intrinsic link between structural liquid heterogeneity and the nucleating ability of templates, which significantly advances our understanding toward the control of nucleation efficiency and polymorph selection.

Automated summary

In this study, we conducted an atomistic investigation of heterogeneous nucleation in Ni using transition path sampling, which revealed a template precursor-mediated mechanism of crystallization. Notably, our findings showed that tiny templates can modify the structural features of the liquid and facilitate the formation of precursor regions with enhanced bond-orientational order, thus determining their nucleation efficiency and the polymorphs that crystallize. These results establish an intrinsic connection between structural liquid heterogeneity and the nucleating ability of templates, significantly advancing our understanding of nucleation efficiency and polymorph selection.