An overview over computational studies of AS-ALD making use of the intrinsic reactivity differences between GS and NGS is found in Tab. 2. The vast majority of studies in this field use computational approaches to explain the experimentally observed selectivity for a given precursor or a set of precursors. Thereby, precursor adsorption on GS and NGS is mostly investigated with DFT approaches (research question (RQ): 1a, 1b in Tab. 2) with one study using a kMC ansatz in addition. Mostly, thermodynamic as well as kinetic driving forces were investigated but in some cases an analysis was based on thermodynamic driving forces alone or the kinetic driving forces were estimated via the BEP relationship. The slab approach was used in most studies. But for modelling of silicon surfaces, cluster approaches with different terminations (bare, H, OH, NH2, Cl, SiH3) are still common until today. Nearly all studies with slab approaches used the PBE density functional (one used PW91). Cluster approaches mostly relied on hybrid density functionals (B3LYP, M06-2X) with one exception of a GGA functional (B97-D). Some cluster calculations used double-zeta basis sets (def2-SVP, LanL2DZ) while the mostly used triple-zeta basis sets (def2-TZVP, 6-311G+(d,p)) are generally recommended for DFT energy computations. The cutoff energy for slab calculations (which determines the accuracy of the basis set in PBC computations) varied depending on the surface modelled from 300-500 eV while some studies do not report this value. As computational codes, VASP is used exclusively for slab calculations, while GAUSSIAN is used for clusters with one exception (NWCHEM ). The reporting of electronic energy differences (ΔE) is the standard, while some studies used ab initio thermodynamics or statistical thermodynamics approaches to consider the finite temperature and pressure under ALD conditions (ΔG). Only one study combined the DFT investigations with kMC simulations for packing predictions.