with 5-fold cross-validation for each nucleus across the training set. Full details are provided in the SI. The achieved predictions of CQ , η, θ, and ϕ for all Li in the test set are compiled in Fig. , with comparable findings for the other two nuclei, as well as results for the MAE(V ij ) provided in the SI. CQ and η show an acceptable correlation between DFT and ML data. The Pearson correlation for CQ and η is r = 0.96 and r = 0.84, and the MAE is 0.17 and 0.14, respectively. In contrast, the predictions of θ and ϕ are of a substantially lower quality, with no visible linear trend in the correlation plots shown in Fig. . This is reflected in the corresponding poor Pearson correlations of r = 0.46 and r = 0.28, and MAEs of 0.47 and 0.75 radians, for θ and ϕ, respectively. This corresponds to a staggering MAE of 27 • for θ and 43 • for ϕ.