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The rotational and translational diffusion of negatively charged and uncharged spin probes in five imidazolium-based room-temperature ionic liquids (RTILs), 1-ethyl-3-methylimidazolium tetrafluoroborate, emimBF4, 1-butyl-3-methylimidazolium tetrafluoroborate, bmimBF4, 1-octyl-3-methylimidazolium tetrafluoroborate, omimBF4, 1-octyl-3-methylimidazolium hexafluorophosphate, omimPF6, and 1-octyl-3-methylimidazolium chloride, omimCl, has been studied by means of electron paramagnetic resonance spectroscopy. Detailed analyses of the spin-Hami