We have characterized the magnetic and structural properties of the CdLn 2 Se 4 (Ln = Dy, Ho), and CdLn 2 S 4 (Ln = Ho, Er, Tm, Yb) spinels. We observe all compounds to be normal spinels, possessing a geometrically frustrated sublattice of lanthanide atoms with no observable structural disorder. Fits to the high temperature magnetic susceptibilities indicate these materials to have effective antiferromagnetic interactions, with Curie-Weiss temperatures Θ W ~ -10 K, except CdYb 2 S 4 for which Θ W ~ -40 K. The absence of magnetic long range order or glassiness above T = 1.8 K strongly suggests that these materials are a new venue in which to study the effects of strong geometrical frustration, potentially as rich in new physical phenomena as that of the pyrochlore oxides.
1The geometry of the lanthanide ion sublattice in the pyrochlore structure is an array of corner sharing tetrahedra based on kagomé planes that connect via triangular layers. This arrangement of spins can show geometric frustration, such that no long range magnetic ordering occurs, even at low temperatures. 1,2 The magnetic behavior of the Ln 2 Ti 2 O 7 pyrochlores is widely studied, and, despite weak coupling between structural and magnetic degrees of freedom, the rare earth pyrochlores exhibit a particularly rich range of magnetic behavior due to a balance between dipole interactions, single ion anisotropy, and exchange couplings. 3,4,5,6,7,8,9 Many of these materials possess strong crystal fields causing highly anisotropic spin states. In Dy 2 Ti 2 O 7 and Ho 2 Ti 2 O 7 the spins' directionality and effective ferromagnetic interactions produce Ising-like spins leading to spin ice characteristics, where the orientations of the spins are analogous to the H positions in ice. 10,11,12,1314,15,16,17,18,19,20,21,22 We characterized the sample structures through x-ray powder diffraction data using CuKα radiation and a diffracted beam monochromater. Structural refinements were made using the Bruker AXS software package TOPAS 2.1 © operated with a Pseudo-Voight TCHZ fitting profile. Refined parameters include: zero corrections; sample displacement; scaling factors; cell dimensions; atomic positional coordinates; and 3 thermal parameters (B eq ). We measured the d.c. magnetic susceptibility with a SQUID magnetometer (Quantum Design MPMS) on cooling over T = 290 -2 K in an applied field of H = 0.1 T. We also performed measurements of a.c. magnetic susceptibility using the ACMS option for a Quantum Design PPMS cryostat. This instrument also gives d.c. magnetization measurements in fields up to 9 tesla using an extraction method.Curie-Weiss fits to the d.c. susceptibility data performed over T = 80 -270 K, with the exception of CdYb 2 S 4 , where fits were performed between T = 250 -350 K. The applied field dependence of the magnetization was measured at selected temperatures for all materials up to a field of 7 Tesla.Structure refinement shows all samples to be normal spinels with lattice parameters similar to those found previously 32,35,36 . ...