The starting materials and reagents used to assemble the reactions are known compounds, and their NMR spectra are either reported or can be immediately acquired. In such cases, we used reported or experimental spectra to refine the predicted spectra for these reaction components. To adjust the NMR parameters (isotropic shifts, J -couplings, and Gaussian FWHM broadenings), the simulated spectrum was fit to the experimental spectrum using the python package Mrsimulator . Mrsimulator increases the accuracy of NMR parameters calculated by DFT, and this approach resulted in better fitting with the HMCMC procedure.