With a view to establishing high-throughput computations, static models of the cages had been used. A downside of this approach is that it effectively ignores entropic contributions and is rather an analysis of the enthalpy of the systems. As such, when entropic considerations dominate the selfassembly process, 23e,43 this approach may not be appropriate. It became clear that fundamental components of the models necessary for qualitative reproduction of experimental results were being overlooked. It is anticipated that interactions with solvent and counterions, and conformational flexibility, also play significant roles. The precise manner of these, and their relative impact on individual systems, however, remains unknown. Without a clear indication of how such additional interactions might be reliably incorporated into the models at this stage, further studies were abandoned.