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Ionic liquids (ILs) are appealing electrolytes for their favorablephysicochemical properties. However, despite their longstanding use,understanding the capacitive behavior of ILs remains challenging. This islargely due to the formation of a non-conventional electric double layer (EDL)at the electrode-electrolyte interface. This study shows that the short-rangeYukawa interactions, representing the large anisotropically charged ILs, demixIL to create a spontaneous surface charge separation, which is reinforced bythe strongly coupled charge interaction. The properties of the condensed layer,the onset of charge separation, and the rise of overscreening and crowdingcritically depend on the asymmetry of Yukawa interactions.

Electric Double Layer from Phase Demixing Reinforced by Strong Coupling Electrostatics