The growth dynamics of faceted three-dimensional (3D) Ag islands on weaklyinteracting substrates are investigated-using kinetic Monte Carlo (kMC) simulations and analytical modelling-with the objective of determining the critical top-layer radius required to nucleate a new island layer as a function of temperature T, at a constant deposition rate. kMC shows that decreases from 17.3 to 6.0 Å as T is increased at 25 K intervals, from 300 to 500 K. That is, a higher T promotes top-layer nucleation resulting in an increase in island height-to-radius aspect ratios. This explains experimental observations for film growth on weakly-interacting substrates, which are not consistent with classical homoepitaxial growth theory. In the latter case, higher temperatures yield lower top-layer nucleation rates and lead to a decrease in island aspect ratios. The kMC simulation results are corroborated by an analytical mean field model, in which is estimated by calculating the steady-state 2 adatom density on the island side facets and top layer as a function of T. The overall findings of this study constitute a first step toward developing rigorous theoretical models, which can be used to guide synthesis of metal nanostructures, and layers with controlled shape and morphology, on technologically important substrates, including two-dimensional crystals, for nanoelectronic and catalytic applications.
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