Emergence of quadrupolar order under magnetic field in $5d^2$ double perovskites

Abstract

Motivated by the time-reversal symmetry breaking signal in muon spin relaxation below a transition temperature without accompanying noticeable magnetic Bragg peaks in $5d^2$ Os double perovskites, a rare ferro-octupolar order was proposed to account for such hidden order. Here we study the phase transitions under a magnetic field in triangular and face-centered cubic lattices using classical Monte Carlo simulations. It is expected that higher-rank moments do not couple linearly to the magnetic field. Consequently, a field applied along the ferro-octupolar order is not anticipated to influence the ordering. However, we observe the emergence of antiferro-quadrupolar ordering mixed with the antiferro-octupolar order (AFQO) due to the field-induced bond-dependent exchange interaction. This field-linear interaction among non-Kramer doublets arises via the coupling to the excited triplet states enabled by the external field. In the triangular lattice, we uncover intriguing vortex states, which could inspire future research into $5d^2$ triangular lattice systems.