Interplay of superexchange and vibronic effects in the hidden order of Ba$_2$MgReO$_6$ from first principles

TL;DR

This study uses first-principles calculations to reveal how intertwined exchange and vibronic couplings give rise to the hidden quadrupolar and magnetic orders in Ba$_2$MgReO$_6$, challenging traditional explanations.

Contribution

It introduces an ab initio low-temperature effective Hamiltonian that incorporates both electronic exchange and vibronic couplings to explain the hidden order.

Findings

Quadrupolar hidden order is resilient under pressure.

Uniaxial strain rapidly suppresses the hidden order.

Intertwined exchange and electron-lattice couplings drive the order.

Abstract

The origin of the "hidden" quadrupolar and unconventional magnetic low-temperature orders observed in the spin-orbit double perovskite Ba$_2$MgReO$_6$ 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 $J_{eff}=3/2$ 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 Ba$_2$MgReO$_6$ and similar $d^1$ double perovskites.