Physical properties of R$_2$Co$_6$Al$_{20-\delta}$ (R = Gd-Tm, Y) single crystals

Abstract

Rare-earth (R) based intermetallic compounds can often exhibit diverse physical properties and distinct magnetic anisotropies. A Notable example are the light rare earth members of the mono-clinic, R$_2$Co$_6$Al$_{19}$ series that are known to display a range of physical properties, from non-Fermi liquid behavior to antiferromagnetic (AFM) ordering, with properties that vary depending on R. In this work, we have extended this series to the heavy rare earths and systematically investigate the synthesis, crystal structure, and physical properties of single crystals of R$_2$Co$_6$Al$_{20-\delta}$ for R = Gd - Tm and Y. Single crystal X-ray diffraction reveals that these materials adopt an orthorhombic Imma-type structure with delta varying non-monotonically across the heavy rare earths; ranging from 0.73 for Dy to 0.91 for Gd. Temperature-dependent specific heat, resistivity, and magnetization measurements demonstrate AFM ordering in all materials, with the Neel temperature (TN) ranging from 1.8 K for Ho to 11.8 K for Tb. Notably, Gd and Tb-based materials exhibit two distinct AFM transitions, separated by approximately 2 - 3 K. These findings establish the heavy rare-earth members of the R2Co6Al20-delta series as anisotropic antiferromagnets with strong crystal electric field effects and exchange anisotropy. The observed deviation from de Gennes scaling and the anisotropy crossover across the series highlight the important interplay between RKKY exchange and crystal electric field interactions in this orthorhombic system.