To obtain the E σiσj and E σi,σj parameters, we fit eq. 1 to a set of known energies of NPs with different chemical orderings by means of linear regression. The NP energies are calculated by means of the Effective Medium Theory (EMT) approach as implemented in the asap calculator of the Atomic Simulation Environment . This allows testing and validating results using large data sets obtained at very low computational cost. Calculations based on Density-Functional Theory (DFT) are also used to validate the most important results obtained in this work and to show the general applicability of our approach to obtain DFT-like accuracy while using a dataefficient strategy. Details regarding the accuracy of the topological energy expression and the DFT calculation parameters are described in the Supporting Information (Fig. ).