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The radical anion of aceneazulenedione in which a benzoquinone is fused to an azulene moiety was generated by electrolysis and by reduction with the alkali metals in ethereal solvents. The hyperfine data could not be reproduced by standard Hückel calculations which usually give reliable predictions for the spin distribution in radical ions such as azulene quinones and a variety of extended π systems. However, PPP and, preferably,ab initio geometry optimisations followed by single-point calculations of the Fermi contact interaction with density functional theory, led to a straightforward assignment of the hyperfine coupling constants.

applied magnetic resonance

Application of quantum-chemical methods including density functional theory for the interpretation of isotropic hyperfine data. The example of azulenebenzoquinone