The cut-off for CG pair-wise interactions was set to 10 Å. As the CG model had uniaxial symmetry, only the position and out-of-plane principal axis of each molecule were needed to define the pair interaction. To scale the torque residual in Eq. ( ) in the CG parametrization, we took η = 1.63 Å, the average semi-axis length of benzene, but the optimized CG potential was found to be largely insensitive to the choice of this scaling factor (see section SIV E of the SM). Following optimization of the CG potential, the root-meansquare error (RMSE) between the CG and FG forces (the square root of the force residual in Eq. ( )) was 2.58 kcal mol -1 Å-1 , while the RMSE for the torque was 4.66 kcal mol -1 .