In our analysis, we have deliberately neglected the disorder of the linker, because its effect on the DS signal is weak. However, in the 3D-∆PDF [Fig. , there is some weak evidence for correlations between the internode distances, which emerges due to correlations between the node orientation and the linker. Understanding these correlations is complex, as they depend on the orientation of both the node and the linker. Instead of modelling this disorder and comparing to data, we take a theoretical approach to understanding this linker relaxation in response to the orientations of the SBUs it is bound to. More specifically, we use the experimentally derived oxygen positions for the ferro-and antiferrohexapolar node orientations to constrain a density functional theory (DFT) optimisation of the linker geometry. The details of this simulation are given in the S.I.