Switchable slow relaxation of magnetization in the native low temperature phase of a cooperative spin-crossover compound
The implementation of single-molecule magnet properties in spin crossover materials is sought as a unique source of magnetic multistability at the molecular level. Examples however remain extremely scarce, in part due to the diamagnetic state of most Fe( II ) spin crossover materials at low temperatures. We have studied the complex [Fe(mtz) 6 ](CF 3 SO 3 ) 2 (mtz = 1-methyltetrazole) as a tantalizing candidate of such coexistence, due to its known partial spin crossover and therefore paramagnetic native low temperature phase. The single-crystal structures of [Fe(mtz) 6 ](CF 3 SO 3 ) 2 reported here allow rationalizing its peculiar cooperative spin-crossover behavior. Importantly, the high-spin Fe crystallographic sites at low temperature exhibit a high symmetry with a local trigonal distortion, usually source of magnetic anisotropy. The analysis of equilibrium magnetic properties confirm the presence of a significant magnetic anisotropy at the Fe( II ) high spin sites in the high symmetry low temperature phase. This results in field-induced slow relaxation of their magnetization which is dominated at low temperature by tunneling and direct processes and is strongly enhanced above 3 K by Raman and Orbach processes. Unprecedentedly, these single-molecule magnet properties are observed in the native ground state of a spin crossover material and efficiently and reversibly switched OFF through visible light irradiation.