We began by studying the series of simple, hydrogen-substituted o-phenylenes on the left of Chart 1. 1 H NMR spectra were acquired at 273 K as the signals were slightly sharper below room temperature, as is typical for o-phenylenes. As shown in Figure (top) and ). It is clear from comparison with the behavior of the known parent hepta(ophenylene) that the assignments are consistent with "perfect" folding into a compact helix analogous to that shown in Figure . For example, H 4b , H 1a , H 2e , and H 3e , highlighted in Figure , are all highly shielded compared to typical aromatic protons. In the folded state, these protons are all placed directly in the shielding zones of nearby aromatic rings.