Spin Density Distribution and Interaction Mechanisms in Thiazyl-based Magnets

This chapter presents a study of the magnetic properties and magnetic interaction mechanisms in a series of thiazyl radicals, which are of particular interest in the field of molecular magnetism. The chapter is organized as follows. First, there is an introduction to organic molecular magnetism and thiazyl radicals. The importance of an accurate knowledge of the spin density distribution in order to understand the mechanisms of the magnetic interactions is discussed. This is highlighted with complimentary experimental and theoretical ab initio determinations of the spin density distribution in the dithiadiazolyl radical, p-O2NC6F4CNSSN. An ab-initio computation of the magnetic interactions in this radical is presented in relation to its spin density distribution and magnetic behaviour. This approach is then extended to other dithiadiazolyl and thiazyl radicals. Finally, the conclusions revealed from this study are summarized.