Spin-orbit-entangled frustrated magnetism in fcc Ba$_2$(Yb,Nd)NbO$_6$ double perovskites

Abstract

The search for candidate Kitaev materials has largely focused on 4$d$ and 5$d$ transition-metal compounds with various lattice geometries. In contrast, investigations of rare-earth 4$f$ systems have thus far been restricted mainly to honeycomb and triangular lattices. In this work, we investigate the rare-earth-based double perovskites Ba$_2$YbNbO$_6$ and Ba$_2$NdNbO$_6$, which crystallize in a face-centered cubic structure. Magnetization and heat-capacity measurements establish isolated ${j_{\rm eff}} = 1/2$ Kramers doublet ground states arising from strong spin-orbit coupling (SOC) and crystal electric-field effects, which are further supported by density-functional theory calculations. Millikelvin-temperature thermodynamic measurements reveal long-range magnetic order with moderate frustration in both compounds. The emergence of magnetic order may be understood within an order-by-disorder scenario, as theoretically proposed for rare-earth fcc lattices with finite Kitaev interactions. Our results thus identify Ba$_2$YbNbO$_6$ and Ba$_2$NdNbO$_6$ as promising rare-earth spin-orbit-entangled magnets and motivate further experimental and theoretical investigations aimed at determining the complete exchange tensor to elucidate the microscopic origin of the underlying magnetic interactions.