In order to maximize the coverage of different regions of the PES, the set was generated from 10 high mutation rate GA instances with the GAFF force field, and with the structures that resulted from GA crossovers and mutations before local relaxations (and fitness evaluations). Therefore, these latter are not LM of the GAFF force field which is only used to drive the sampling. From all visited configurations (20000 in total), 200 diverse geometries were initially selected using a farthest-point sampling (FPS) algorithm 102 in the space defined by the radius of gyration RG and the number of hydrogen bonds NH (see Appendix 6.2) that turned out to be useful for differentiating polypeptide configurations. 103 Among these, 146 geometries were successfully relaxed to distinct LM at the B3LYP/6-31G(d,p) reference level, which we augmented with 42 structures derived from ab initio SA (cf. Section 2.1) that we know correspond to low energy minima. Hence, the test set finally contains 69 cis and 119 trans non-relaxed individuals that are representative of points potentially visited during GA runs.