Quantum criticality in a uniaxial organic ferroelectric

TL;DR

This study investigates quantum criticality in a uniaxial organic ferroelectric, revealing a persistent quantum critical regime and unexpected dielectric behavior due to ultra-weak dipoles, with implications for ferroelectric applications.

Contribution

First detailed investigation of quantum criticality in a uniaxial organic ferroelectric, showing deviations from theoretical predictions due to ultra-weak dipoles.

Findings

Quantum critical regime persists up to 30-40K.

Dielectric susceptibility varies as 1/T^2 instead of 1/T^3.

Ultra-weak dipoles explain the observed dielectric behavior.

Abstract

Tris-sarcosine calcium chloride (TSCC) is a highly uniaxial ferroelectric with a Curie temperature of approximately 130K. By suppressing ferroelectricity with bromine substitution on the chlorine sites, pure single crystals were tuned through a ferroelectric quantum phase transition. The resulting quantum critical regime was investigated in detail - the first time for a uniaxial ferroelectric and for an organic ferroelectric - and was found to persist up to temperatures of at least 30K to 40K. The nature of long-range dipole interactions in uniaxial materials, which lead to non-analytical terms in the free-energy expansion in the polarization, predict a dielectric susceptibility varying as $1/T^3$ close to the quantum critical point. Rather than this, we find that the dielectric susceptibility varies as $1/T^2$ as expected and observed in better known multi-axial systems. We explain this result by identifying the ultra-weak nature of the dipoles in the TSCC family of crystals. Interestingly we observe a shallow minimum in the inverse dielectric function at low temperatures close to the quantum critical point in paraelectric samples that may be attributed to the coupling of quantum polarization and strain fields. Finally we present results of the heat capacity and electro-caloric effect and explain how the time dependence of the polarization in ferroelectrics and paraelectrics should be considered when making quantitative estimates of temperature changes induced by applied electric fields.