The correlation between the magnetic properties and crystal structure of is
ostructural pi-d interaction systems (C1TEX-TTF)FeBr4 (X=S, Se) is investig
ated by crystal structure analysis and magnetic susceptibility measurements
. These salts form a sheet structure consisting of one-dimensional anion zi
gzag chains and donor dimers, the latter of which bridge between two anion
chains. The susceptibility, to which only Fe3+ (S=5/2) spins contribute as
a triangle-based spin ladder system, shows antiferromagnetic phase transiti
ons at T-N=4.2K and 3.6K for X=S and Se, respectively Below T-N, weak ferro
magnetism appears due to the Dzyaloshinski-Moriya interaction when the fiel
d is applied along one of the spin hard-axes. The difference between the tw
o salts in the weak ferromagnetic transition suggests that the interaction
between two Fe3+ spin ladders is reduced by a half with changing X=S to Se.