An X-ray crystal structure of the methylbenzodithiazolyl radical MeC6H3S2N,
MBDTA, reveals that it forms a regularly spaced pi-stack motif in the soli
d state; variable temperature magnetic studies show that the susceptibility
passes through a broad maximum at 140 K indicative of exceptionally strong
antiferromagnetic coupling for an organic radical possessing extended magn
etic interactions. Its behaviour can be modelled as a two-dimensional Heise
nberg square lattice of S = 1/2 ions with J = -72 K.