  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.
