We next aimed to quantify the geometric and electronic structure characteristics of the three key trajectories for which Asp1 in TC10b has a large charge coupling with the previously identified residues (i.e., Asp4, Lys8, and Ser20). To confirm these charge couplings were not a consequence of the method of cross-correlation analysis , we also computed the mutual information between the charge distributions (Figure ). Indeed, we observe high mutual information values for these three trajectories between Asp1 and the respective residues (Figure ). This observation holds despite the fact that geometric couplings are modest or weakly anticorrelated for the same residues over each of these trajectories (Figure ). Thus, it appears that charge coupling captures interactions between Asp1 and proximal residues (i.e., Ala4) as well as more distant residues (i.e., Ser20 or Lys8). The same observations can be made from the full SQM trajectory (Supporting Information Figure ). To elucidate what structural orientations give rise to this coupling, we next computed the distributions of charges and identified extrema for these three pairs of residues (i.e., Asp1 with Ala4, Lys8, or Ser20). A wide distribution of both QM residue charges is observed, with variations on the order of 0.4 a.u., regardless of whether the residue is neutral (i.e., Ala4) or charged (i.e., Lys8 or Ser20, Figure ). These charge distributions are comparable to those we had previously observed in small proteins for charged residues but larger than the typical charge distributions we had noted for most neutral residues (i.e., non-polar or polar). The greater statistics in SQM trajectories lead to an apparently narrower distribution of charges but are otherwise consistent with our QM observations (Supporting Information Figure ). Focusing on the most extreme cases in the charge distributions reveals which structures favor a more positive charge on Asp1 versus a more negative charge (Figure ). In the trajectories for which Lys8 or Ala4 coupling are strongest, Asp1 in the most extreme cases takes on a weakly positive charge (Figure ). In the Asp1-Lys8 structure, a salt bridge is observed between the sidechain of the residues (Figure ). For all three trajectories, the most negative charge on Asp1 occurs when it is distant from the paired residue, forming no interactions and thus having a net charge as low as -0.4 a.u.. In the case of Asp1-Ser20, this orientation appears stabilized by a salt bridge between the N-terminal and C-terminal backbone atoms (Figure ). Thus, very strong couplings between sequence-distant residues can arise due to dynamic hydrogen-bonding interactions.