RESUMO
Interfacial adsorption of solute atoms is a promising means to tune heterogeneous nucleation. In this study, a new method has been established to theoretically evaluate the effect of solute addition on the nucleation potency of heterogeneous nucleation interfaces. The evaluation consists of three steps: (1) analyzing the solute adsorption behavior; (2) determining the nucleation mode; and (3) evaluating the effect of solute adsorption on nucleation potency using the solute-adsorbed interface model. A combination of the ab initio and molecular dynamics methods together with the two-phase thermodynamic model was used to evaluate a prototype Al-Cu/(0001) sapphire interface. It is found that solute Cu atoms adsorb at the interface between the melt and (0001) sapphire interface. The adsorption is driven by the strengthening of the Cu-Al bonds as revealed by the Bader charge analysis which is demonstrated to reduce interfacial energy. Furthermore, it is revealed that the interfacial adoption of Cu results in the formation of an Al-Cu adsorption layer, which enhances the interfacial chemical affinity thus enlarging the nucleation driving force. Meanwhile, the lattice mismatch between the sapphire substrate and the primary Al (α-Al) nucleus is decreased by Cu addition, which lowers the barrier for nucleation. The above two effects together increase the nucleation potency of the studied interface, which is in good agreement with previous experiments. It is proposed that the effect of solute adsorption shall be considered in the search for effective substrates for tuning the nucleation.
