Direct simulations of 2 H NMR spectral lineshapes and T1 relaxation times, using methodology previously applied to EPR spectra, clearly show that the MD simulations fully capture the dynamics observed in NMR, and the both the lineshape and relaxation can be explained by the same processes occurring on fast (ns) timescales. Crucially both libration and jump-type motions are treated on an equal footing, avoiding trying to fit lineshapes purely in terms of jump-type models. This explains why traditional approaches to interpreting 2 H NMR data gave inconsistent and misleading results, even though good fits could be obtained with individual experimental data sets.