As an extension to our work done with xTB we demonstrate the feasibility of using py-GlobOpt with a DFT software as its energetic evaluator. We perform 3000 DFT LO calculations on Pt NPs at various stages of hydrogenation with and without our tuned settings (c.f. section 3.3.5). We only LO to the relatively high 0.3 eV/ Å to save time and allow the majority of the finer optimisation to be performed by the GO algorithm, this increases the structure number and reduces the time spent on trying to optimise particularly difficult structures. We perform 500 pyGlobOpt iterations per run as this is enough to demonstrate the proof of concept. We acknowledge, given our prior results, this will likely only capture a small portion of the low energy PES. We can estimate this proportion using the xTB PES in section 3.5. Assuming the PESs are similar in terms of their energy distribution of local minima of Pt 13 H 4 , and that the ULES discovery rate is the same when using this energetic driver with optimal settings, from figure (top) we would expect to find 18.5±9.27 ULES in this run out of a possible 1290 structures. However, we would expect those ULES to skew disproportionately towards the lower energy, and therefore more ensemble relevant, part of the energy distribution profile. We take our GM for these structures to be the lowest found across each stoichiometries for all runs performed.