All DFT calculations for this work were conducted with the ORCA quantum chemistry package in version 5.0.4 or 6.0.0. If not stated otherwise, the DFT functional for all q-vSZP comparisons is ωB97X-D4. The resolution of the identity (RI) approximation for the electronic Coulomb energy with the large universal auxiliary basis sets by Weigend as well as seminumerical chain-of-spheres approximation for the Fock exchange were used throughout. For numerical derivatives, high convergence thresholds (keyword: VeryTightSCF) and grid settings (keyword: DefGrid3) were applied to exclude numerical noise to the extent possible. The D4 parameters employed with the (revised) q-vSZP basis set were taken from the original publication in Ref. Like in the first version, geometry optimizations are conducted with numerical energy derivatives, fully adapting the basis set for each distorted geometry. All numerical derivatives with respect to nuclear coordinates or external electric fields were conducted with the help of an in-house Python code, which is publicly available within the corresponding GitHub repository (). Geometry optimizations were conducted with the ANCopt optimizer in xtb,