Interplay of superexchange and vibronic effects in the hidden order ofBa2⁢MgReO6from first principles

Abstract

The origin of the “hidden” quadrupolar and unconventional magnetic low-temperature orders observed in the spin-orbit double perovskite Ba2⁢MgReO6 defies explanation through standard experimental and theoretical techniques. Here we address this problem by deriving and solving an ab initio low-temperature effective Hamiltonian including intersite electronic exchange and vibronic (electron-lattice) couplings between 𝐽eff=3/2 Jahn-Teller-active rhenium states. Our findings disclose the nature of these elusive states, attributing it to intertwined exchange and electron-lattice couplings, thus diverging from the conventional dichotomy of purely electronic or lattice driving mechanisms. Our results indicate the resilience of the quadrupolar hidden order under pressure, yet its rapid suppression under uniaxial strain suggests that external or lattice-induced distortions play a pivotal role in determining the relative stability of competing phases in Ba2⁢MgReO6 and similar 𝑑1 double perovskites.