Two kinds of molecular design for genuinely organic molecule-based ferrimag
netics are reported. (I) The coulombic interaction between an anion and a c
ation is utilised for co-crystallizing organic radical molecules with diffe
rent spin quantum numbers. This is referred to "organic salt ferrimagnetics
". A phenol derivative of nitronyl nitroxide pi -biradical with S=1 has bee
n synthesised as an anionic component of the salt and the electronic spin s
tructure characterized. (II) The phenolic pi -biradical with S=1 and a carb
oxyl-substituted pi -radicals with S=1/2 have been esterified to give model
compounds for "single-component ferrimagnetics". Potentialities of the mod
el compounds as building blocks of molecule-based ferrimagnetics have been
examined by susceptibility and ESR measurements.