Dipolar and quadrupolar correlations in the 5⁢𝑑2 Re-based double perovskites Ba2⁢YReO6 and Ba2⁢ScReO6

Abstract

Double perovskites containing heavy transition-metal ions are an important family of compounds for the study of the interplay between electron correlation and spin-orbit coupling. Here, by combining magnetic susceptibility, heat capacity, and neutron scattering measurements, we investigate the dipolar and quadrupolar correlations in two prototypal rhenium-based double perovskite compounds Ba2⁢YReO6 and Ba2⁢ScReO6. A type-I dipolar antiferromagnetic ground state with a propagation vector 𝐪=(0,0,1) is observed in both compounds. At temperatures above the magnetic transitions, a quadrupolar ordered phase is identified. Weak spin excitations, which are gapped at low temperatures and softened in the correlated paramagnetic phase, are explained using a minimal model that considers both the dipolar and quadrupolar interactions. At larger wave vectors, we observe dominant phonon excitations that are well described by density functional calculations.