A particular advantage of the Green function approach is that thinner surface models are needed to obtain fully converged surface energies and work functions. For electrochemical system, the Green function approach is the only currently available method which allows direct control over the bulk Fermi level; because the semiconductor bulk Fermi level is an input to the model, as in the case of GC-DFT, the Green function method guarantees that the relevant bulk Fermi level is used as the absolute electrode potential (Eq.( )). It has also been shown that the method can model e.g. band bending, the SCR, and surface states at different dopant concentrations and as a function of the Fermi level. Despite these attractive features, the method has not, however, been applied to study SCEs. We believe that this is because the method requires the use of a localized (LCAO) basis set and has only been implemented in the proprietary QuantumATK software used mainly in the semiconductor industry. Currently, dielectric electrolyte models have not been included in QuantumATK, which limits the use of the Green function method for SCEs. Finally, implementing both localized orbitals and the Green function method in widely used plane wave DFT codes would require significant development work.