AIMD trajectories are produced at 333 K by means of the CP2K software , starting from a cubic box of 17.52 Å formed by 16 ChCl ion pairs and 16 LAs produced by CMD simulations. NVT ensemble calculations are performed using the Nose-Hoover ther-mostat . A production of 109 ps is obtained, with a time step of 0.5 fs, at the BLYP-D3/DZVP-MOLOPT-SR-GTH level. Due to the higher computational cost associated with AIMD calculations, several CMD simulations are carried out containing 16 molecules of each molecular compound. This allows for a direct comparison of results between the two levels of theory. In this case, the CMD simulations involve 2 ns of equilibration time followed by 10 ns of production time. The size and time convergence aspects of these calculations are further discussed in the supplementary material (section S1).