Equilibration simulations were done under NPT conditions with a time step of 2 fs using GROMACS. A mass rescaling method for the backbone hydrogen atoms is employed to enable using larger time steps during MD equilibration. A 1.0 nm cutoff for Lennard-Jones and electrostatic interactions was used and all nonbonded interactions for 1-2 and 1-3 bonded pairs were excluded and a scaling factor of 0.5 was used for 1-4 bonded pairs. V-rescale thermostat and C-rescale barostat were used for packing steps and the Nose-Hoover thermostat and Parrinello-Rahman barostat were employed for equilibration runs. Verlet cutoff scheme was employed for non-bonded interactions and Particle-mesh Ewald was used for long-range electrostatic interactions. Examples of coordinate, topology, and run files can be found in . We previously verified the quality of the models generated by the workflow shown in scheme 1 and equilibrated through "melt" method for IDT-BT, where a strong agreement between the simulated X-ray scattering patterns from our models and the pattern given by GIWAXS measurement was achieved, see Figure in ref. Similar analyses on the microstructures of two DPP-based (i.e., DPP-2TT and DPP-DTT) and two BT-based (i.e.. IDT-BT and TIF-BT) models obtained from "melt" equilibration has been done and a comparison with experimental data is discussed in section 2.2 of the SI, demonstrating that a single workflow can be successfully validated across a class of materials.