A Markov State Modelling analysis, which has previously been applied mainly to protein dynamics, was successful in identifying stable states, pathways between them and corresponding transition rates. This analysis provided direct insight into slower larger amplitude motions (as distinct from faster motions such as libration), identifying two main states for ethanol within the FSPA structure, and four symmetry-equivalent states for acetone. This two-fold and four-fold degeneracy is consistent with the local molecular and crystallographic symmetry. It is important to note, however, that this insight cannot be obtained from comparing predicted and experimental NMR data, since the 2 H quadrupolar tensor is under inversion and so inversion-type dynamics will be invisible to 2 H NMR. This weakness is shared with classic approaches to modelling 2 H lineshapes using Markov jump-models, where a simplistic model based on C2 jumps provides a satisfactory (but ultimately incorrect) fit to the experimental data (cf. Figure ).