Abstract
This chapter explains zero-field splitting (ZFS) in the context of single-molecule magnets (SMMs). It provides information on high-frequency and high-field electron paramagnetic resonance (HFEPR). Both the period of the electron paramagnetic resonance (EPR) transitions and their spread on the field scale are proportional to the magnitude of the zero-field splitting (ZFS), a phenomenon characteristic for all high-spin systems of sufficiently low symmetry. ZFS offers a very important spectroscopic window into the electronic structure of mononuclear. The chapter explains how ZFS and g-tensor values are determined using HFEPR. It also explains why HFEPR is indispensable for investigating high-spin mononuclear transition metal complexes. HFEPR spectra, when properly analyzed, yield the spin Hamiltonian parameters D, E, and g values; in some cases they yield the full g matrix, in others, only one or two of the three components. The chapter then explains in detail how both kinds of parameters, ZFS and g-tensor values are determined using HFEPR.
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