Of course, this modelling strategy based on partial optimizations can be coupled to other automated conformational search methods from the very beginning , or even MD simulations to obtain the candidate structures. In fact, after analyzing the MD trajectories, some interaction pattern isomers listed in Table could not be identified using the procedure described above. To address this, we conducted a second round of conformational sampling post hoc, starting from a set of C/d structures classified as the missing conformers. Still, some isomers could not be optimized, but they can be safely ignored because their low populations make their overall contribution to the spectrum negligible. The effect of expanding the aggregate set on the Q/s populations and the computed IR spectra is discussed in the SI (see Section E).