Abstract
The paramagnetic behavior of 18-electron cyclopentadienylnickel(II) complexes of the [CpNi(μ-Br)]2 type with two unpaired electrons per metal ion has been investigated by 1H and 13C NMR spectroscopy of [Cp‴Ni(μ-Br)]2 (1; Cp‴ = 1,3,4-tBu3C5H2), [3CpNi(μ-Br)]2 (2; 3Cp = 1,3,4-iPr3C5H2), and [4CpNi(μ-Br)]2 (3; 4Cp = 2,3,4,5-iPr4C5H). The tri-tert-butylcyclopentadienyl derivative 1 crystallizes in the triclinic space group P1 and has been investigated by X-ray crystallography. Solid-state magnetic susceptibility measurements of 3 revealed an effective magnetic moment at room temperature of 4.04 μB, confirming the presence of two d8 nickel(II) ions. While antiferromagnetic coupling via the bromo bridges is weak (J = −2.4 cm–1), zero-field splitting is substantial (D = +48.2 cm–1). NMR spectra of complexes 1–3 show signals with half-widths up to 3600 Hz within a spectral window exceeding 500 ppm (1H) or 2200 ppm (13C). An analysis of the spectra gave insight into the spin delocalization, the equilibrium orient...
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