DFT simulations access the limit of {t p , t d } ! 0, as in Equations 4 and 5, and neglect any experimental dead time, hence allowing us to naturally simulate a nonensemble averaged ACF ! Q for site specific trajectories within a molecular dynamics (MD) simulation. We can therefore target processes which are faster than the lower limit of what is possible in experimental SAE, as the experiment is limited by the lower bound on the order of 10 µs, defined by t d and t p as well as the inverse of the quadrupolar interaction . It is therefore possible to extract an atomistic ACF ! Q from an MD simulation as long as one can calculate the EFG tensors for all Li atoms across every snapshot of the simulation. A single snapshot of the MD simulation with ! Q and C Q calculated for each individual atomic site from DFT is the equivalent of the 0 K temperature limit, in which all motion in the system is frozen and all ions remain in their initial site. Under realistic room temperature experimental conditions for SAE, the quadrupolar observables are averaged ( CQ and !Q ), not only over the fast timescale hopping events which are masked in experiment but also over thermal effects and different Li sites. for LPS to the final training of the UFP (B) and ML-EFG model (C). The UFP has an RMSE in the energies of 3.1 meV/atom and forces of 109.9 meV/Å . The ML-EFG model is assessed both by the quality of the relative orientation of the tensors and the MAE in !Q. C shows the combined distribution function (CDF) of the quaternion scalar product between the DFT and ML quaternions, q DFT • q ML . This indicates that the majority of tensors are oriented in the same direction comparing DFT to ML. The ML-EFG model has an error of 7.4 kHz on !Q, where the experimental sensitivity of 7 Li SAE is shown shaded in red, as 10 kHz for !Q.