This section now summarizes the contributions that computational modeling can make to the field of AS-ALD. It is interesting to note that it is often stated that ALD needs multiscale modelling to be understood. However, the microscopic aspects (e.g., surface chemistry) can be treated quite independently from the macroscopic aspects (e.g., gas flow) which explains the success of many DFT-based approaches in ALD. This is all the more the case for AS-ALD modeling, where selectivity is mostly determined by the local reactivity of precursors and inhibitors on GS and NGS. Although recent approaches exist to extend to multiscale modeling, the necessity in the framework of modelling AS-ALD is still an open question. As outlined in the introduction, the focus here is thus on the insights gained by ab initio modelling of the key aspects of AS-ALD. A comprehensive overview of studies in AS-ALD that contain computational investigations is found in Tab. 1 for inhibitor-based approaches and in Tab. 2 for intrinsically selective approaches. This includes studies which focus on a theoretical investigation of certain aspects as well as the vast majority of studies where experimental data are either explained by computations or where predictions from computations are checked experimentally. Notably, the details on the computational approaches are often found only in the supporting information of the studies cited.