Across all three approaches, we employed the same method to generate a coordinate block. Specifically, we created the Gen3Molecules dataset with coordinate sections for random small molecules and selected one of them randomly. This dataset consists of valid molecules with up to three atoms and was created from random SELFIES, followed by conversion to SMILES. The Cartesian coordinates were then generated with rdkit. We opted for small molecules with up to three atoms because this dramatically reduces simulation times while allowing for the full range of ORCA simulations (except for dihedral angle constraints). Notably, we also generated radicals to support open-shell methods such as unrestricted Hartree-Fock calculations. However, we excluded ions and heavy atoms like bromine and iodine.