Electronic Absorption Spectra and Electronic Structures of Some Würster’s Blue Salts

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Abstract
Electronic absorption spectra were measured at various temperatures for Würster’s blue iodide, bromide, and chloride. The charge-transfer bands were found to be strongly dependent upon temperature. Concerning the iodide, the temperature dependency can be explained quantitatively, or at least semiquantitatively, by the aid of the linear Ising model in relation to the local ordering of the electron spins of Würster’s blue cation radicals. This model gives the exchange energy of 99±23 cm−1 for the iodide. For the bromide and the chloride, the dimer model was successfully applied to the analysis of the temperature dependence of the charge-transfer bands, giving singlet-triplet energy separations of 248±30 cm−1 and 255±30 cm−1 for the bromide and the chloride, respectively. The electronic structure and the intermolecular interaction were discussed for these radical salts, their electronic absorption spectra being compared with one another.

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