The reaction of Co(NCS)2withN-methylaniline
leads to the formation of [Co(NCS)2(N-methylaniline)2]n(1), in which
the cobalt(II) cations are octahedrally coordinated and linked into
linear chains by pairs of thiocyanate anions. In contrast to [Co(NCS)2(aniline)2]n(2) reported recently, in which the Co(NCS)2chains
are linked by strong interchain N–H···S hydrogen
bonding, such interactions are absent in1. Computational
studies reveal that the cobalt(II) ions in compound1show an easy-axis anisotropy that is lower than in2, but with the direction of the easy axis being similar in both compounds.
The high magnetic anisotropy is also confirmed by magnetic and FD-FT
THz-EPR spectroscopy, which yield a consistentgzvalue. These investigations prove that the intrachain interactions
in1are slightly higher than in2. Magnetic
measurements reveal that the critical temperature for magnetic ordering
in1is significantly lower than in2, which
indicates that the elimination of the hydrogen bonds leads to a weakening
of the interchain interactions. This is finally proven by FD-FT THz-EPR
experiments, which show that the interchain interaction energy in
theN-methylaniline compound1is nine-fold
smaller than in the aniline compound2.