Considering the smaller number of atoms in simulation box, the extremely faster equilibration, and the exemption of Tg calculation for "soup" method, obtaining 250 independent samples for QC calculations takes on average one tenth of the computation time needed for the "melt" method. It should be noted that we used 20 annealing cycles for equilibration through "melt" approach to cover a homogenous setting for all polymers in this study (see SI, section 2.2); however, the number of cycles needed for different polymers varies based on their relaxation time spectra and needed to be determined each individual polymer by monitoring its properties during equilibration. This shows another advantage of the "soup" method, for which we use one simulation setting for any polymer at hand without monitoring its properties during equilibration. In Table , we summarised the computational cost, including the force field generation, MD equilibration, and QC calculations, for the "melt" and "soup" methods to achieve the same statistical sampling. In fact, this analysis shows that by employing the workflow for SCP model generation (shown in scheme 1), the calculation (including the investigator) time has been tremendously decreased (from typically a few months per polymer per investigator to below two weeks per polymer per computer node) so that the "melt" method is reasonably suitable to investigate electronic structure properties of any polymer of interest as well as several polymers in one investigation. Moreover, the "soup" method (with total calculation time of around 1-2 days per polymer per computer node) can be pushed to become a discovery tool where a large number (e.g., hundreds) of hypothetical models are explored in one study. Table . The computational time of "melt" and "soup" QC/MD methods considering the five SCPs discussed in this paper. Note that similar GPU-and CPU-computer nodes (one Nvidia A40 GPU/AMD EPYC 7443 CPU and one Intel(R) Xeon(R) Gold 6230, for MD and QC calculations, respectively) were used for all polymers through "melt" and "soup" methods.