The compound [Fe(tvp)(2)(NCS)(2)]. CH3OH, where tvp is 1,2-di-(4-pyrid
yl)-ethylene, has been synthesized and characterized by x-ray single-c
rystal diffraction. It consists of two perpendicular, two-dimensional
networks organized in parallel stacks of sheets made up of edge-shared
[Fe(II)](4) rhombuses. The fully interlocked networks define large sq
uare channels in the [001] direction. Variable-temperature magnetic su
sceptibility measurements and Mossbauer studies reveal that this compo
und shows low-spin to high-spin crossover behavior in the temperature
range from 100 to 250 kelvin. The combined structural and magnetic cha
racterization of this kind of compound is fundamental for the interpre
tation of the mechanism leading to the spin crossover, which is import
ant in the development of electronic devices such as molecular switche
s.