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Relevant academic research and scientific papers

Disjoint and coextensive diradical diions

N,N,N',N'-Tetraanisyl-3,3'-diaminobiphenyl and N,N,N',N'-tetraanisyl-3,3'-diaminobiphenyl have been synthesized and their oxidations studied by cyclic voltammetry and EPR spectroscopy.A two-electron oxidation of the former species gives a ? system which is disjoint and oxidation of the latter gives a ? system which is coextensive.Cyckic voltammetry is shown to be a useful tool for reveaaling the difference between the disjoint and coextensive ? systems.The coulombic contribution to the difference between the half-wave potentials for the first and second oxidation steps (ΔE), which measures the 'hole-hole' repulsion energy, was extracted by measuring δE as a function of the relative permittivity of the medium.This was substantially greater in the coextensive case.Both diradical diions gave triplet EPR spectra.A comparison of the cyclic voltammetry of N,N,N',N'-tetraanisyl-3,3'-diaminobiphenyl and that of a high-spin polymer precursor with the same local topology showed that, in the oxidized polymer, the additional hole-hole repulsion energy associated with the coextensive spin-spin distribution is of the order 0.1-0.2 V-a noticeable effect but not one large enough to explain the difficulties that have been encounted in achieving high doping levels in this and related high-spin polymers.