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Whereas the majority of ions in the bulk of a solvent-free ionic liquid isbound into clusters, this is expected to change in the electrical double layer(EDL), in which the resulting electric field 'prefers' to interact withelectrical monopoles-free, unclustered ions. The competition between thepropensity of ions to stay in a clustered state and the reduction of the energyof ions in electric field in the free state determines the resulting portion offree ions in the EDL. We present a study of this effect, based on the simplestpossible mean-field theory. 'Cracking' of ion clusters into individual ions inelectric field is accompanied by the change of the dielectric response of ionicliquid which is different in clustered and unclustered states. The predictionsof the theory are verified and further explored by specially performedmolecular dynamics simulations. A particular finding of the theory is that thedifferential capacitance vs potential curve displays a bell shape despite lowconcentration of free charge carriers, because the dielectric response of boundions reduces the threshold concentration of the bell- to camel-shapetransition. Whereas qualitatively these findings make perfect sense, in realitythe exact numbers and criteria might be different as the presented simpletheory does not take into account overscreening and oscillating charge andelectrostatic potential distributions near the electrode. This is why testingthe theory with computer simulations is essential, but the latter basicallyreproduce the qualitative conclusions of the theory.

Enforced freedom: electric-field-induced declustering of ionic-liquid ions in the double layer