In recent contributions, it was demonstrated that the anisotropy of π‐electron density could be considered as a reliable descriptor to probe the aromaticity in a wide range of annulene and hetero‐monocyclic compounds. The electron density anisotropy on a plane can be simply measured by the ratio of two in‐plane Hessian eigenvalues associated with the eigenvectors lying in the plane. This descriptor is undirected and has a circular symmetry for aromatic rings, whereas it is directed and has an elliptical shape in antiaromatic cycles. This research takes a step forward towards the extension of this approach to polycyclic conjugated hydrocarbons. The obtained results show that the anisotropy of the π‐electron density works nicely for the assessment of local aromaticity in polycyclic compounds. This finding provides clear evidence to have a universally successful aromaticity descriptor based on the topological properties of one‐electron density distribution.
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