Abstract

We present an $S=2$ antiferromagnet composed of a Mn-verdazyl complex $[\mathrm{Mn}{(\mathrm{hfac})}_{2}]\phantom{\rule{0.16em}{0ex}}[o\text{\ensuremath{-}}\mathrm{Py}\text{\ensuremath{-}}\mathrm{V}\text{\ensuremath{-}}{(4\text{\ensuremath{-}}\mathrm{F})}_{2}]$. An analysis of the magnetic behavior reveals that the strong antiferromagnetic intramolecular interaction between spins on ${\mathrm{Mn}}^{2+}$ and the verdazyl radical forms an $S=2$ hybrid spin below approximately 100 K. In the low-temperature regions, the magnetic susceptibility and the specific heat indicate a phase transition to the three-dimensional order of the $S$ = 2 system. Below the transition temperature, the magnetization curve exhibits a metamagnetic phase transition. From the analysis of electron spin resonance modes, we evaluate the on-site biaxial anisotropy responsible for the anisotropic magnetic behavior.

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