Interplay of superexchange and vibronic effects in the hidden order of Ba₂MgReO₆ unravelled from first principles

The origin of the "hidden" quadrupolar and unconventional magnetic low-temperature orders observed in the spin-orbit double perovskite Ba₂MgReO₆ 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 inter-site 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 Ba₂MgReO₆ and similar d¹ double perovskites.