Combined experimental and theoretical study of hydrostatic (He-gas) pressure effects in $\alpha$-RuCl$_3$

TL;DR

This study combines experimental measurements and theoretical calculations to understand how hydrostatic pressure affects the structure and magnetism of $ ext{α-RuCl}_3$, revealing pressure-induced phase transitions and magnetoelastic coupling.

Contribution

It provides a comprehensive analysis of pressure effects on $ ext{α-RuCl}_3$, including the first detailed correlation between structural transitions and magnetic properties under pressure.

Findings

Pressure suppresses magnetic ordering temperature $T_N$ from 7.3 K to 6.1 K.

A structural transition occurs at pressures above 104 MPa, causing Ru-Ru bond dimerization.

Magnetic susceptibility increases with pressure before dimerization, indicating enhanced magnetic response.

Abstract

We report a detailed experimental and theoretical study on the effect of hydrostatic pressure on the structural and magnetic aspects of the layered honeycomb antiferromagent $\alpha$-RuCl$_{3}$. Magnetic susceptibility measurements performed under almost ideal hydrostatic-pressure conditions yield that the phase transition to zigzag-type antiferromagnetic order at $T_N$ = 7.3 K can be rapidly suppressed to about 6.1 K. A further suppression with increasing pressure is impeded due to the occurrence of a pressure-induced structural transition at $p \geq$ 104 MPa, accompanied by a strong dimerization of Ru-Ru bonds, which gives rise to a collapse of the magnetic susceptibility. Whereas the dimerization transition is strongly first order, as reflected by large discontinuous changes in $\chi$ and pronounced hysteresis effects, the magnetic transition under varying pressure and magnetic field also reveals indications for a weakly first-order transition. We assign this observation to a strong magnetoelastic coupling in this system. Measurements of $\chi$ under varying pressure in the paramagnetic regime ($T > T_N$) and before dimerization ($p <$ 100 MPa) reveal a considerable increase of $\chi$ with pressure. These experimental observations are consistent with the results of ab-initio Density Functional Theory (DFT) calculations on the pressure-dependent structure and the corresponding pressure-dependent magnetic model. Comparative susceptibility measurements on a second crystal showing two consecutive magnetic transitions instead of one, indicating the influence of stacking faults. Using different temperature-pressure protocols the effect of these stacking faults can be temporarily overcome, transforming the magnetic state from a multiple-$T_N$ into a single-$T_N$ state.