Most notably, the EnS (Figure ) demonstrated excellent performance from the BestCCR starting point, with minimal additional improvement needed during subsequent optimization steps. The good performance of the parametrization is reflected in the PES descriptions for both CCR-IRC and DHFR-SC data sets (Figures and, respectively), where the reparametrized GFN2-xTB closely matches the reference M06-2X-D3/def2-TZVP calculations.