We
proposed the concept of atomic layer modulation (ALM) based
on precursor chemical reactivities and steric hindrance effects to
fabricate multicomponent nanofilms. Because ALM employs consecutive
precursor exposures followed by exposure to a counter reactant, the
composition of ALM films is determined by the molecular size and chemical
reactivities of the precursors. For the demonstration, dicarbonyl-bis(5-methyl-2,4-hexanediketonato)Ru(II) (Carish) and trimethylaluminum
(TMA) were used as Ru and Al precursors, respectively, and H2O was used as the counter reactant. Prior to the experiments, the
chemical reactivity and sterically hindered physisorption of the Ru
and Al precursors were theoretically calculated using density functional
theory (DFT) and Monte Carlo (MC) simulations, respectively. The transmission
electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS)
results were highly consistent with the theoretical results, and the
growth characteristics were well explained by the MC- and DFT-based
reaction models. We believe that ALM could be extended to other material
systems, thereby providing a different method of fabricating multicomponent
nanofilms for various applications including semiconductors and nanodevices.