After we appended the coordinate block, we ran the generated ORCA input to see whether it is executable, ensuring they represent valid data. Importantly, for executable files, we replaced the coordinate block with a comment containing the SMILES of the molecule. We did this because generating meaningful Cartesian coordinates with LLMs is challenging as they consist solely of floating-point numbers. Since tools like rdkit readily generate valid coordinates, training an LLM for this would be inefficient. Additionally, we believe that LLMs would not be suited for that. By including the SMILES, we focused instead on teaching the model to associate certain basis sets with specific elements.