For comparison, the ADMM error in selected angles of the optimized ES geometries is depicted in Figure , demonstrating that the impact of the chosen auxiliary basis on the angles is less dependent on the basis set size than it is for the bond lengths even though the width of the Gaussian distribution is reduced when going from double to triple-zeta basis sets. An analogous plot for the GS, given in the SI, looks nearly identical with the only difference that outliers with maximum errors in the angles rising up to 18.9 • and 7.9 • are found for the C C C and C C H angles of the dzp structures of cyanoacetylene. For the dzp basis, the ES of this molecule is thus predicted to be significantly less bent in comparison to auxiliary basis sets with larger cardinal numbers as well as the conventional PBE0 results with a DZVP, TZVP and TZV2P primary basis. Outliers were checked to confirm they are local minima, but further characterization of the excited state would be needed to draw final conclusions. However, smaller angles, as predicted by the dzp auxiliary basis, are in better agreement with EOM-CCSD and experimental reference data -an agreement which might be due to fortuitous error cancellation.