Quantum-mechanical calculations for morphology analysis. We performed singlepoint density functional theory (DFT) calculations (B3-LYP 27 /def2-SV(P) level of theory as implemented in Turbomole 29 ) of each PEDOT conformer extracted from the last snapshot of all MD trajectories. We chose a charge of 2+ for each PEDOT oligomer which allows us to interpret the energy of the highest occupied molecular orbital as the approximate energy of an additional third hole on the PEDOT chains, which is the typical charge of PEDOT oligomers when being ionized by PSS chains at the PEDOT:PSS ratio assumed in this work. The electronic couplings were calculated using DFT (B3-LYP/def2-SV(P)) using a frontier (HOMO) orbital based diagonalization method. Fock and overlap matrices were extracted from PEDOT dimer calculations and HOMO orbitals were extracted from calculations of isolated PEDOT molecules.