The coupled cluster data set was created using the same geometries as those in the DFT calculations. Energies and forces were recomputed employing all-electron CCSD(T). The Dunning's correlation-consistent basis set cc-pVTZ was utilized for ethanol, cc-pVDZ for toluene and malonaldehyde, and CCSD/cc-pVDZ for aspirin. All calculations were executed with the Psi4 software suite. Data Accessibility: All data sets are available at datasets. The rMD17 data set can also be accessible on Figshare at . In addition, all data sets are provided as a class in the PYG library.[123]