The interpolation errors for a Fe simulation dataset are on par with the intrinsic uncertainty of the dataset itself (Section S3.1). Analysis of the GPR fitting results indicates that the Ni and Fe simulation datasets have correlation lengths of 8.3°and 7.4°, respectively, but that when the Ni dataset is constrained to have low noise, the numerical correlation length drops to ∼1.9°. Plotting of geodesic paths between low-Sigma GBs of interest reveal that a Σ7 cusp has a monotonically de-creasing path towards the coherent-twin Σ3 cusp, whereas a Σ5, Σ9, and Σ11 cusps do not necessarily share this same type of monotonically decreasing path within a VFZ. We demonstrated that two cusps can be connected in 5DOF space.