Focusing on these first two singlet and triplet excitations, the above shown six properties relating to their energies and (if applicable) oscillator strengths were extracted to serve as labels for training ML models. Here, notebook "02" was used to interactively probe for optimal CV-grid settings for each label on a coarse grid of size 16 × 16 at first. The finally chosen parameters and an example output of ArchOnML's hyperparameter optimization are given in the ESI sections S2.6 and S3.2.