See the supplementary material for detailed information on the asphaltene monomers, the change in angle between monomer TDMs after dimer structure optimization, comparison of DFT functionals, estimation of BSSE, S1 and diabatic state energy and excited state EDA result for the different conformers of the rotated C22-PC113 and C05-C22 dimers, monomer ID used in Figure and Figure , energy and excited state EDA for the TDM-perpendicular C22-X series, S1 composition analysis for the TDM-perpendicular C22-X series, monomer ID used in Figure and Figure , and results for excited state EDA and S1 composition analysis of 496 coal asphaltene dimers (PDF).