The computed geometries for Li2 [1-3] agreed well with the experimentally determined solid-state XRD structures respectively, including the ~30° twist of the aryl substituents relative to the pentalenide core in 2 and 3. To elucidate the degree of aromaticity in the conjugated π systems of arylated pentalenides, we calculated the anisotropy of the induced current density (ACID) as well as nucleusindependent chemical shift (NICS) scans along different axes across the molecules (as indicated in the insets in Figures ).