“…Imidazolium cations are known to collectively reorientate to parallel alignment with respect to the electrode surface under cathodic applied potentials. 44,70,71 Such reorientation aligns imidazolium cations with each other and reduces the average distance between the imidazolium charge center and electrode surface, which together may contribute to the efficient assembly of imidazolium and better stabilization of surface adsorbed molecules under cathodic applied potentials. Particularly, [EMMIm] + , with smaller ring substituents, would undergo the reorientation more easily and exhibit more ordered assembly compared to [EM 4 Im] + , leading to stronger interfacial electric fields.…”