Cooperative cluster-Jahn-Teller effect as a possible route to antiferroelectricity

Abstract

We report the observation of an antipolar phase in cubic GaNb${}_4$S${}_8$ driven by an unconventional microscopic mechanism, the cooperative Jahn-Teller effect of Nb${}_4$S${}_4$ molecular clusters. The assignment of the antipolar nature is based on sudden changes in the crystal structure and a strong drop of the dielectric constant at $T_{\mathrm{JT}}=31$\,K, also indicating the first-order nature of the transition. In addition, we found that local symmetry lowering precedes long-range orbital ordering, implying the presence of a dynamic Jahn-Teller effect in the cubic phase above $T_{\mathrm{JT}}$. Based on the variety of structural polymorphs reported in lacunar spinels, also including ferroelectric phases, we argue that GaNb${}_4$S${}_8$ may be transformable to a ferroelectric state, which would further classify the observed antipolar phase as antiferrolectric.

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Cited by in corpus (9)

• Dynamic Jahn-Teller effect in the strong spin-orbit coupling regime
• Quasimolecular $J_{\mathrm{tet}}$=3/2 moments in the cluster Mott insulator GaTa${}_4$Se${}_8$
• Antipolar transitions in GaNb${}_4$Se${}_8$ and GaTa${}_4$Se${}_8$
• Cluster rearrangement by chiral charge order in lacunar spinel GaNb${}_4$Se${}_8$
• Resonating holes vs molecular spin-orbit coupled states in group-5 lacunar spinels
• Monitoring Vibrational Evolution in Jahn-Teller Effect by Raman Imaging
• Bond Ordering and Molecular Spin-Orbital Fluctuations in the Cluster Mott Insulator GaTa${}_4$Se${}_8$
• Jahn-Teller driven quadrupolar ordering and spin-orbital dimer formation in GaNb${}_4$Se${}_8$
• Optical, dielectric, and magnetoelectric properties of ferroelectric and antiferroelectric lacunar spinels