Orbital-Order Driven Ferroelectricity and Dipolar Relaxation Dynamics in Multiferroic GaMo$_4$S$_8$

TL;DR

This study investigates the complex dielectric relaxation dynamics of GaMo$_4$S$_8$, revealing how orbital-driven ferroelectricity and Jahn-Teller transitions influence dipolar behavior in this multiferroic material.

Contribution

It provides the first broadband dielectric spectroscopy analysis of GaMo$_4$S$_8$, highlighting the distinct dipolar and orbital relaxation mechanisms above and below the Jahn-Teller transition.

Findings

Above T_JT, coexistence of relaxor-like and order-disorder dynamics.

Below T_JT, long-range ferroelectric order with domain dipolar dynamics.

Differences in relaxation behavior compared to GaV$_4$S$_8$ linked to structural distortions.

Abstract

We present the results of broadband dielectric spectroscopy of GaMo$_4$S$_8$, a lacunar spinel system that recently was shown to exhibit non-canonical, orbitally-driven ferroelectricity. Our study reveals complex relaxation dynamics of this multiferroic material, both above and below its Jahn-Teller transition at T$_{\textrm{JT}}=47$ K. Above T$_{\textrm{JT}}$, two types of coupled dipolar-orbital dynamics seem to compete: relaxations within cluster-like regions with short-range polar order like in relaxor ferroelectrics and critical fluctuations of only weakly interacting dipoles, the latter resembling the typical dynamics of order-disorder type ferroelectrics. Below the Jahn-Teller transition, the onset of orbital order drives the system into long-range ferroelectric order and dipolar dynamics within the ferroelectric domains is observed. The coupled dipolar and orbital relaxation behavior of GaMo$_4$S$_8$ above the Jahn-Teller transition markedly differs from that of the skyrmion host GaV$_4$S$_8$, which seems to be linked to differences in the structural distortions of the two systems on the unit-cell level.