Journal
JOURNAL OF PHYSICAL CHEMISTRY B
Volume 119, Issue 23, Pages 7015-7029Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acs.jpcb.5b01093
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- U.S. Department of Energy, Office of Basic Energy Sciences, Division of Chemical Sciences, Geosciences, and Biosciences [DE-SC0008644, DE-FG02-12ER16363]
- U.S. Department of Energy (DOE) [DE-SC0008644] Funding Source: U.S. Department of Energy (DOE)
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The deviations from Stokes Einstein hydrodynamics of small solutes are mote pronounced in ionic liquids than in conventional solvents (J. Phys. Chem. B 2013 117 (39), 11697). Small neutral solutes diffuse much faster than expected, whereas small charged solutes diffuse much slower: This article attempts to establish a link between the local friction experienced by tracer solutes and the polar/apolar structure of ionic liquids. We find that small neutral solutes probe locally stiff (mostly charged, high electrostriction) regions and locally soft (mostly apolar, low eIectrostriction) regions. These regions of high and low friction are associated with cage and jump regimes. Enhanced neutral tracer mobility in the low friction regions associated with the cationic apolar component has an important bearing on the large positive deviations from Stokes Einstein behavior. In contrast, diminished charged tracer mobility involves long caging dynamics separated by jump events often triggered by the loss and recovery of counterions.
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