For the remaining anionic organic bases, gaining spectral resolution revealed additional peaks in the spectra. In the case of KO t Bu and KHMDS, these could be accounted for by including a hyperfine interaction to a single I=3/2 nuclear spin (Figure & S20, Table . K 93% abundance). In an attempt to force the formation of separated ion pairs and reveal the signature of bare [1 •-], we employed chelating agents. When adding the [2.2.2] cryptand (L 1 ), both KO t Bu and KHMDS spectra simplified even further and no hyperfine to K + was needed (Figure and Table ). This was confirmed by single crystal XRD data, which revealed a distance between [K(L 1 )] + and [1 •-] of ~6 Å (Figure , section S2 and Table ), in agreement with Kochi's data (CSD entry EWOCUO) -note that Kochi's structure was obtained by metal reduction, yet we obtain virtually the same crystalline structure. However, employing 15-Crown-5 ether (L 2 ) with KHMDS does not result in a separated ion pair (Figure ), since chelation is expected to occur in the perpendicular plane to nitrobenzene. The situation is more complicated for LiO t Bu and all the sodiumbased Lewis bases, as either one (Figure , S12, S13 & S14), two (Figure & S11) or three (Figure , S4, S5 & S8) I=3/2 nuclear spins are needed to reproduce the spectra. Still, some clarity is gained when using 15-Crown as the number of Na + ions is decreased from three to one for NaO t Bu (Figure vs S9) and from two to one for NaHMDS (Figure vs S12). The fact that at least one ion is always needed to describe these spectra is ascribed to the employed L 1 and L 2 not being efficient at disrupting [1 •-]⋯[Na + ] interactions. Finally, we note that for NaO t Bu there remain some satellite peaks that cannot be fully reproduced with a single Na + ion (Figure ), which is likely originated from small fractions of higher nuclearity compounds still present in solution. For LiO t Bu, using 12-Crown-4 (L 3 ), which is the most appropriately sized crown for Li + , still yields spectra that need three ions, suggesting that the formation of