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Electric Double Layer from Phase Demixing Reinforced by Strong Coupling Electrostatics

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