Jahn-Teller effect in $j=3\mathrm{/}2$ Mott insulators: Ground states and thermal fluctuations

The interplay of strong atomic spin-orbit coupling with Jahn-Teller (JT) lattice distortions is an important theme in quantum materials hosting heavy atoms. A prototypical example of such a system is a degenerate $j=3\mathrm{/}2$ multiplet coupled to local phonon modes. Here, we study the multipolar ground states of this system as realized in Mott insulators, explore its thermal phase diagram via an $SU(4)$ spin Monte Carlo approach coupled to JT phonons, and study the temperature dependent splittings of the $j=3\mathrm{/}2$ multiplet as relevant to spectroscopic probes. Our work sheds light on coexisting distinct multipolar orders engendered by phonon coupling, role of thermal JT fluctuations, and the entropy of the coupled multipole-phonon system. We discuss broad implications for double perovskites $\mathrm{B}{\mathrm{a}}_2\mathrm{M}\mathrm{g}\mathrm{R}\mathrm{e}{\mathrm{O}}_6$, $\mathrm{B}{\mathrm{a}}_2\mathrm{N}\mathrm{a}\mathrm{O}\mathrm{s}{\mathrm{O}}_6$ and lacunar spinels such as $\mathrm{G}\mathrm{a}\mathrm{T}{\mathrm{a}}_4\mathrm{S}{\mathrm{e}}_8$ and $\mathrm{G}\mathrm{a}\mathrm{N}{\mathrm{b}}_4\mathrm{S}{\mathrm{e}}_8$.