The chemistry at the interface between GS and NGS, and its implications for selectivity-reducing reactions, remains largely unexplored. Similarly, nucleation and overgrowth of SMI layers have received limited attention. The targeted removal of inhibitor layers has yet to be addressed through computational studies. While molecular layer deposition has been used in an area-selective manner, computational modeling offers further opportunities for insights beyond the previously discussed use of indicone as an inhibitor layer. Publishing results that do not align with experiments could also provide valuable insights into the limitations of current modeling approaches, despite challenges in dissemination. For intrinsically selective AS-ALD, the influence of precursor dimerization remains unexamined, where differences in the reactivity of monomeric and dimeric forms could help distinguish between two surfaces, e.g., one able to open the dimer and the other not. The integration of density functional theory (DFT) with kinetic Monte Carlo (kMC) simulations is a promising yet unexplored approach. Additionally, while the penetration of precursors and inhibitors into self-assembled monolayer (SAM) layers has been briefly addressed, comprehensive computational investigations remain lacking.