Anisotropic magnetization and transport properties of RAgSb<sub>2</sub> (R=Y, La-Nd, Sm, Gd-Tm)

Abstract

This study of the RAgSb2 series of compounds arose as part of an investigation of rare earth intermetallic compounds containing antimony with the rare earth in a position with tetragonal point symmetry. Materials with the rare earth in a position with tetragonal point symmetry frequently manifest strong anisotropies and rich complexity in the magnetic properties, and yet are simple enough to analyze. Antimony containing intermetallic compounds commonly possess low carrier densities and have only recently been the subject of study. Large single grain crystals were grown of the RAgSb2 (R=Y, La-Nd, Sm, Gd-Tm) series of compounds out of a high temperature solution. This method of crystal growth, commonly known as flux growth is a versatile method which takes advantage of the decreasing solubility of the target compound with decreasing temperature. Overall, the results of the crystal growth were impressive with the synthesis of single crystals of LaAgSb2 approaching one gram. However, the sample yield diminishes as the rare earth elements become smaller and heavier. Consequently, no crystals could be grown with R=Yb or Lu. Furthermore, EuAgSb2 could not be synthesized, likely due to the divalency of the Eu ion. For most of the RAgSb2 compounds, strong magnetic anisotropies are created by the crystal electric field splitting of the Hund's rule ground state. This splitting confines the local moments to lie in the basal plane (easy plane) for the majority of the members of the series. Exceptions to this include ErAgSb2 and TmAgSb2, which have moments along the c-axis (easy axis) and CeAgSb2, which at intermediate temperatures has an easy plane, but exchange coupling at low temperatures is anisotropic with an easy axis. Additional anisotropy is also observed within the basal plane of DyAgSb2, where the moments are restricted to align along one of the <110> axes. Most of the RAgSb2 compounds containing magnetic rare earths, antiferromagnetically ordered at low temperatures. The ordering temperatures of these compounds are approximately proportional to the de Gennes factor, which suggests that the RKKY interaction is the dominant exchange interaction between local moments. Although metamagnetic transitions were observed in many members of the series, the series of sharp step-like transitions in DyAgSb2 are impressive. In this compound, up to 11 different magnetic states are stable depending on the magnitude and direction of the applied field. The saturated magnetization of these states and the critical fields needed to induce a phase transition vary with the direction of the applied field. Through detailed study of the angular dependence of the magnetization and critical fields, the net distribution of magnetic moments was determined for most, of the metamagnetic states. In DyAgSb2, the crystal electric field (CEF) splitting of the Hund's rule ground state creates a strong anisotropy where the local Dy3+ magnetic moments are constrained to one of the equivalent <110> directions within the basal plane. The four position clock model was introduced to account for this rich metamagnetic system. Within this model, the magnetic moments are constrained to one of four equivalent orientations within the basal plane and interactions are calculated for up third nearest neighbors. The theoretical phase diagram, generated from the coupling constants is in excellent agreement with the experimental phase diagram. Further investigation of this compound using magnetic X-ray or neutron diffraction would be extremely useful to verify the net distributions of moments and determine the wave vectors of each of the ordered states.