Calculations with such an additional orbital alignment step were performed for cc-pV(T,Q)Z and a target accuracy TIGHTPNO. Their results are given in the Supporting Information. However, there is no significant difference to be noticed regarding the SDs and MADs such that either the inconsistent orbital maps are not caused by differently localized orbitals or these inconsistencies are either non-existent or irrelevant for the error in the first place.