The magnetic and crystal structures of the [Ni(dmit)(2)](-) (dmit = 1,3-dit
hiol-1,2-thione-4,5-dithiolate) simple salts with N-alkylated cationic deri
vatives of pyridyl nitronyl nitroxide radical (N-R-PYNN) have been studied.
In the system with p-nBuPYNN (p-N-nbutyl-), [Ni(dmit)(2)](-) is found to f
orm ladder chains similar with those found in p-EPYNN[Ni(dmit)(2)]. The mag
netic susceptibility in this salt shows spin-ladder behavior.