Abstract

AbstractCharge transfer complexes possessing a … DADA … structure with both the donor, D, and acceptor, A, being S = 1/2 radicals may exhibit cooperative magnetic phenomena. The complex [Fe(C5Me5)2]+·[TCNQ]−· exhibits metamagnetic behavior. The similarly structured [TCNE]−· and [C4(CN)6]−· complexes are ferromagnets, whereas the [DDQ]−· salt is a paramagnet. The high temperature magnetic susceptibility obeys the Curie‐Weiss expression with θ = + 30, + 30, and + 3 for the [TCNE]−·, [C4(CN)6]−·, and [TCNQ]−· salts, respectively. The ferromagnetic [TCNE]−· salt exhibits zero field Zeeman split 57Fe Mossbauer spectra with an internal field of 425.6 kOe at 4.23 K. After reviewing the current papers discussing ferromagnetism in molecular (organic) compounds, a qualitative model consistent with the necessary bulk spin alignment required for a ferromagnet is presented.

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