In particular, the GaMD run with the upper bound of the dihedral boost potential yielded the maximum number of initial structures on average as compared to the other five GaMD potential settings (see Supplementary Information). Cumulant expansion to the second order was used for GaMD reweighting. As seen in Figure , GaMD can cover the high energy regions such as the left-handed α-helix region α L on the right side, whereas WE cannot sample it within 50 ns of simulation time. This shows that it can be more beneficial to use GaMD instead of WE to sample the free energy landscape, even for this simple system.