The magnetic behavior of Ni(SCN)2 has been studied at low temperatures
for the first time. A Curie-Weiss fit, chi(M)=C/(T-theta), to the sus
ceptibility between 100 and 300 K yields g = 2.13 +/- 0.01 (S = 1) and
theta = 39.8 +/- 1.4 K. Systematic curvature in chi-1 vs T is evident
, however. Despite the large positive theta Ni (SCN) 2 appears to orde
r antiferromagnetically at T(c) = 52 +/- 1 K, slightly below a maximum
in chi(T) at T(chi(max)) = 57.2 +/- 0.5 K, with chi(max) = 0.0331 +/-
0.0003 emu/mol. The ratio T(c)/T(chi(max)) = 0.91 +/- 0.02 does not s
uggest lower magnetic dimensionality. Magnetization isotherms are line
ar to 16 kG; some features suggesting lower temperature transitions oc
cur. Well above T(c) the susceptibility is analyzed assuming axial and
rhombic crystal field distortions, i.e., D[S(z)2-S(S + 1)/3] and E[S(
x)2-S(y)2] spin Hamiltonian terms, with exchange incorporated in a mea
n field approximation. An extraordinarily large \D/k\ almost-equal-to
1 19 K seems to emerge, a result which is very provisional lacking sin
gle crystal data. A mean field analysis of T(c) and theta yields ferro
magnetic intrachain exchange J1/k = 8.6 +/- 0.5 K and antiferromagneti
c interchain exchange J2/k = - 0.76 +/- 0.4 K. It seems more likely th
at D is negative, but even if it is positive the exchange interaction
is large enough to induce magnetic order at finite T(c) in light of th
eories relating T(c) J, and D.