The types of move allowed in the threshold simulations were molecular translations, rotations, perturbations of unit cell lengths and angles, as well as unit cell volume changes. Cutoffs on each move type (see ESI, Table ) were chosen to give similar energy changes for different move types. Probabilities for each move type were set according to the proportion of the total number of degrees of freedom for each move type, in the same way as in our implementation of basin hopping for CSP. The sampling at each lid energy and total lengths of simulations differs between systems, depending on the number of degrees of freedom and energy window that needed to be covered. In the current work, a fixed number of steps was performed at each lid energy. An adaptive schedule was investigated (see ESI) but due to the difficulty of choosing the convergence criteria, it did not improve the completeness of sampling.