A Pictorial View of Viscosity in Ionic Liquids and the Link to Nanostructural Heterogeneity

Prototypical ionic liquids (ILs) are characterized by three structural motifs associated with (1) vicinal interactions, (2) the formation of positive–negative charge-alternating chains or networks, and (3) the alternation of these networks with apolar domains. In recent articles, we highlighted that the friction and mobility in these systems are nowhere close to being spatially homogeneous. This results in what one could call mechanical heterogeneity, where charge networks are intrinsically stiff and charge-depleted regions are softer, flexible, and mobile. This Letter attempts to provide a clear and visual connection between frictionassociated with the dynamics of the structural motifs (in particular, the charge network)and recent theoretical work by Yamaguchi linking the time-dependent viscosity of ILs to the decay of the charge alternation peak in the dynamic structure function. We propose that charge blurring associated with the loss of memory of where positive and negative charges are within networks is the key mechanism associated with viscosity in ILs. An IL will have low viscosity if a characteristic charge-blurring decorrelation time is low. With this in mind, engineering new low-viscosity ILs is reduced to understanding how to minimize this quantity.