Origin of spin glass magnetic behavior and phase stability of flux-grown RE(Al, Cr, Fe)B4 (RE = Ho and Er) single crystals

Abstract

The YCrB4 type (α-phase, orthorhombic with space group Pbam) α-HoAlB4 and α-ErAlB4 single crystals which were self-flux grown exhibit the spin glass magnetic behavior, which is anomalous compared to the other reported rare earth system phases of α-REAlB4. Local atomic arrangements with the atomic-resolution for α-HoAlB4 and α-ErAlB4 compounds have been investigated by spherical aberration (Cs)-corrected scanning transmission electron microscopy (STEM) with high-angle annular detector dark-field (HAADF) and annular bright-field (ABF), and STEM-energy-dispersive X-ray spectroscopy (EDS) techniques to elucidate the origin of the exotic magnetic behavior. Observed HAADF- and ABF-STEM images and STEM-EDS chemical maps taken with the incident beam parallel to the [001] direction clearly indicate the existence of substitutions for Al atom sites. The phase stability of RAlB4 (R = Ho ∼ Lu) compounds was discussed from the viewpoint of crystallographic features with lattice parameters and compositions. Based on the presented results, it could be concluded that the origin of the spin glass behavior for self-flux grown α-HoAlB4 and α-ErAlB4 single crystals is the unexpected substitution of Cr/Fe atoms for Al ones. Simultaneously, the substitution by Cr/Fe atoms for Al atoms is indicated to play a significant role to stabilize the YCrB4-type α-HoAlB4 and α-ErAlB4 compounds.