Once the classical equilibration was completed, hybrid QM/MM MD simulations (8 in total) were launched, using the QM/MM interface of the CPMD code with GROMOS, employing the QM/MM coupling scheme developed by Rothlisberger et al. In each case, the three DNA base pairs of interest (residues 58-60/233-235 and 87-89/204-206 for regions 1 and 2 respectively) were treated at the Density Functional Theory (DFT) level, using the BLYP functional for the exchange and correlation energies, in combination with Dispersion-Corrected Atom-Centered Potentials (DCACPs) to properly account for dispersion forces. The rest of the system was described with the force fields used in the classical MD. For each residue of the QM region, the QM-MM boundaries were placed at the Finally, it should be mentioned that, as it has already been discussed in detail, redox properties determined with computational schemes as the one employed here can be subject to corrections to ∆A R→O and λ in order to account for contributions due to the finite size of the simulated periodic box and/or to background charge interactions between periodic images when explicit counter ions are not used to neutralize the system. For the NCP systems of this work, given (i) the large size of the simulated periodic box and (ii) the use of Na + and Cl -ions for neutralization, these corrections to the redox properties are negligible.