We compute the LOL isosurfaces for the optimized radical cations of allene and spiropentadiene. Here there is only the helical representation of the frontier MOs, which are shown in Figure along with the LOL isosurfaces. The doubly occupied HOMO of both radical cations are P-helices, while the SOMOs are M-helices. The LOL π-basins are connected by a P-helical topology that matches the doubly-occupied HOMO. This can be seen in the two bifurcation points at the central carbon atoms of allene and spiropentadiene cations, which differ from the four symmetric bifurcation points surrounding their central carbon atoms in the neutral species (Figure ). The electron delocalization in the cation thus has unique helicity associated to it, which is related to the helicity of their frontier MOs. Helical π-conjugation thus manifests itself in the cationic species because an electron with a specific helicity is missing in the SOMO. This helical conjugation provides intuition for why the cationic species of allene and spiropentadiene twist. If we do the computation for the vertical cation with an infinitesimal twist applied, the helicity of the electronic structure shows in the LOL isosurface. In this sense, the radical cations relax in direction of the helical electron delocalization.