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The electronic structure of spiro[4.4]nonatetraene I as well as that of its radical anion and cation were studied li different spectroscopies. The electron-energy-loss spectrum in the gas phase revealed the lowest triplet state at 2.98 eV and a group of three overlapping triplet states in the 4.5-5.0 eV range. as well as a number of valence and Rydberg singlet excited states. Electron-impact excitation functions of pure vibrational and triplet states identified various states of the negative ion, in particular the ground state with an attachment energy tit 0.8 eV. an excited state corresponding to a temporary electron attachment to the 2b, MO at an attachment energy of 2.7 eV. and a core excited state at 4.0 eV. Electronic-absorption spectroscopy in cryogenic matrices revealed several states of the positive ion. in particular a richly structured first band at 1.27 eV, and the first electronic transition of the radical anion. Vibrations of the ground state of the cation were probed by IR spectroscopy in a cryogenic matrix. The results are discussed on the basis of density-functional and CASSCF/CASPT2 quantum-chemical calculations. In their various forms, the calculations successfully rationalized the triplet and the singlet (valence and Rydberg) excitation energies of the neutral molecule. the excitation energies of the radical cation. its IR spectrum, the vibrations excited in the first electronic absorption band, and the energies of the ground and the first excited states of the anion. The difference of the anion excitation energies in the gas and condensed phases was rationalized li a calculation of the Jahn-Teller distortion of the anion ground state. Contrary to expectations based on a single-con figuration model for the electronic states of 1. it is found that the gap between the first two excited states is different in the singlet and the triplet manifold. This finding can be traced to the different importance of configuration interaction in the two multiplicity manifolds.