For each pair, adjacent heavy atoms were selected to complete the sets of Boresch anchor points. These sets were ordered by increasing total variance of the Boresch DoF, as done by Alibay, and sets of anchor points were discarded if the average values of θ A or θ B were below 30 or above 150 degrees. The equilibrium values for all restraints were taken to be their average values during the unrestrained simulation. Force constants were selected so that in the decoupled state, the harmonic restraints would generate the same distributions as observed in the coupled state. Gaussian distributions in the coupled state were assumed and the variances of the Boresch DoF were used to calculate the force constants (Section S7).