Free radical probes of organic conductor constituents: Electronic structures and hyperfine properties

Density functional theory calculations were carried out on the structures, energetics and hyperfine properties of radical Mu adducts to the molecules tetrathiafulvalene (TTF), bis(ethylenedithio)tetrathiafulvalene (BEDT-TTF or ET) and tetracyanoquinodimethane (TCNQ). In TTF and ET molecular rearrangements may be involved in the formation of some of the species observed in μSR experiments. For TCNQ, a theoretical case is given for a radical formation mechanism with an anionic intermediate, although some apparent inconsistencies with experiment remain. Copyright © 2000 John Wiley & Sons, Ltd.