A comparative study of the magnetic properties and magnetic structures of the natrochalcite, NaFe(2)(D(3)O(2))(MoO(4))(2) (FeD) to those of the isostructural NaCo(2)(D(3)O(2))(MoO(4))(2) (CoD) and NaNi(2)(D(3)O(2))(MoO(4))(2) (NiD) is presented. The structural change is a shrinking of the unit cell in the order of the ionic radii of the transition metal, FeD> CoD > NiD. While NiD and CoD are canted-antiferromagnets with T(N) = 28 and 21 K, respectively, FeD is an anisotropic 2D-Ising antiferromagnet (T(N) = 17 K) with a spin-flop field of 14 kOe at 2 K and the presence of a hysteresis loop reaching only (1)/(4) of the saturation magnetization in 70 kOe. The critical field decreases almost linearly on warming to T(N). The neutron diffraction patterns of FeD below T(N) display numerous magnetic Bragg peaks which cannot be assigned to any one magnetic structure but fits well to two superposed sets, one with a temperature independent line width and has a propagation vector k(1) = (0, 0, 0) while for the other there is a clear dependence and k(2) = (0, 0, ½). In the k(1) = (0, 0, 0) magnetic structure the moments are parallel to each other within one chain and lie along the a-axis but are antiparallel to those in neighboring chains. In contrast CoD and NiD, for which k = (0, 0, 0), have their moments aligned along the b-axis and ac-plane, respectively. The second magnetic structure, k(2) = (0, 0, ½), is characterized by four sublattices, two per layer, where the moments are in the ab-plane and canted with a resultant along the a-axis which is compensated by those of the adjacent layers. For the k(2) = (0, 0, ½) structure, the scattering coherent length decreases, and the moments tend progressively toward the a-axis upon increasing temperature. The coexistence of two concomitant magnetic structures is unprecedented for compounds containing transition metal moment carriers.
