Geometry optimization A subset of 48 molecules did not converge using the previously described geometry optimization parameters . This is most likely due to the generated conformer resulting in an unfavorable initial configuration for geometry optimization. The computational framework allows users to adjust key parameters such as basis sets, gradient convergence tolerance, and the maximum number of steps to address convergence challenges. However, our primary focus at this stage is to enable the generation of molecular structures for spectral predictions, rather than achieving high-level molecular optimization. Therefore, users also have the flexibility to employ alternative tools for refining these molecular structures. In this context, we leveraged the xTB code to address the molecular optimization of the aforementioned molecules. Accuracy of predicted spectra A comparison between the predicted and experimentally acquired spectra, based on intensity ratio similarity (cosine score) and the number of matching ions, does not show any direct trend indicating the failure of the method to achieve meaningful predictions, with the scores and ion matches heterogeneously distributed (Figure ).