Neutron diffraction and thermodynamics techniques were used to probe the evolution of the magnetic properties of Tb(CoxNi1−x)2B2C. A succession of magnetic modes was observed as x is varied: the longitudinal modulated k = (0.55, 0, 0) state at x = 0 is transformed into a collinear k = ( 1 /2, 0, 1 /2) antiferromagnetic state at x = 0.2, 0.4; then into a transverse c-axis modulated k = (0, 0, 1 /3) mode at x = 0.6, and finally into a simple ferromagnetic structure at x = 0.8 and 1. Concomitantly, the low-temperature orthorhombic distortion of the tetragonal unit cell at x = 0 is reduced smoothly such that for x ≥ 0.4 only a tetragonal unit cell is manifested. Though predicted theoretically earlier, this is the first observation of the k = (0, 0, 1 /3) mode in borocarbides; our findings of a succession of magnetic modes upon increasing x also find support from a recently proposed theoretical model. The implication of these findings and their interpretation on the magnetic structure of the RM2B2C series are also discussed.PACS numbers: 71.27.+a,75.25.+z, 75.50.Cc,75.30.Fv Rare-earth 4f moments at regular crystalline sites of intermetallic matrices are subjected to a variety of competing interactions, such as the Ruderman-KittelKasuya-Yosida (RKKY), crystalline electric field, magnetoelastic, and dipolar interactions.1,2 A particular class of such 4f intermetallics is the quaternary isomorphous borocarbides RM 2 B 2 C (R is a rare earth or Y, and M is a transition metal), which have been found to exhibit coexistence between superconductivity and magnetism for a judicious choice of R and M .3-8 Apart from the interesting issue of coexistence (which highlights the importance of electron interactions, with themselves as well as with the 4f moments), the magnetic properties of these materials pose a challenging problem in their own right, especially when R is magnetic and M is nonmagnetic. For the interesting case of M = Co or Ni, Table I indicates that, for fixed R, the Co-based members exhibit collinear and equal-amplitude ferromagnetic (FM)/antiferromagnetic (AFM) structures;9-11 by contrast, the Ni-based members exhibit a variety of modulated structures, few equal-amplitude and commensurate AFM structures, and an absence of FM modes.
12Rhee et al.13 have calculated the generalized susceptibility for borocarbides from band structures obtained through the local-density approximation (LDA): for a fixed pair R and M , three incommensurate peaks were predicted near k 1 = (0.6, 0, 0), k 2 = (0, 0, 0.9) and k 3 = (0, 0, 0.3). Though calculated for the nonmagnetic LuNi 2 B 2 C, the results were expected to be valid for all R, with the precise position and sharpness of each peak depending on R and M . Experimentally, both k 1 and k 2 modes show up in HoNi 2 B 2 C and, moreover, k 1 is evident in, for example, R = Er, Tb, Gd (Ref.12) but, so far, k 3 has not been observed in borocarbides. It is recalled that this model does not account for many modes [e.g. Ref. 13, the authors attributed this to the fact that their theory ...