A comprehensive variable temperature, pressure and frequency multinuclear (H-1, H-2, and F-19) magnetic resonance study was undertaken on selectively deuterated 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl) amide (BMIM TFSA) ionic liquid isotopologues. This study builds on our earlier investigation of the effects of increasing alkyl chain length on diffusion and dynamics in imidazolium-based TFSA ionic liquids. Fast field cycling H-1 T-1 data revealed multiple modes of motion. Through calculation of diffusion coefficient (D) values and activation energies, the low- and high-field regimes were assigned to the translational and reorientation dynamics respectively. Variable-pressure H-2 T-1 measurements reveal site-dependent interactions in the cation with strengths in the order MD3 > CD3 > CD2, indicating dissimilarities in the electric field gradients along the alkyl chain, with the CD2 sites having the largest gradient. Additionally, the alpha saturation effect in T-1 vs. P was observed for all three sites, suggesting significant reduction of the short-range rapid reorientational dynamics. This reduction was also deduced from the variable pressure H-1 T-1 data, which showed an approach to saturation for both the methyl and butyl group terminal methyl sites. Pressure-dependent D measurements show independent motions for both cations and anions, with the cations having greater D values over the entire pressure range. (C) The Author(s) 2017. Published by ECS. All rights reserved.