AS-ALD modeling is nearly exclusively based on DFT computations. It is well-known that these efficient ab initio method has limited accuracy. Furthermore, this accuracy can hardly be quantified intrinsically (exceptions are intrinsic error estimates in some functionals like BEEF-vdW ) and requires benchmarking to experimental data. However, these experimental data are hardly available. The second option for assessing the accuracy, the comparison to highly accurate wavefunction-based methods, is only available for the computation of molecular aspects of AS-ALD like the dimerization of precursors. An option not yet well explored in AS-ALD modeling is the usage of more modern density functionals (e.g., the B97 family) , which promise an overall increase in accuracy. Also, the usage of converged computational parameters (e.g., basis sets and cluster sizes in cluster-based studies) will add to the increased accuracy of computational results. Besides the accuracy of the electronic energy computations, it is also necessary to have a look at the accuracy of thermodynamic modeling. For the calculation of Gibbs energies, it is important to consider ALD conditions in the derivation of correction terms. Moreover, moving beyond the harmonic approximation is a challenging but potentially promising avenue here.