Abstract

Magnetic properties of the substitution series Ru$_{1-x}$Cr$_x$Cl$_3$ were investigated to determine the evolution from the anisotropic Kitaev magnet $\alpha$-RuCl$_3$ with $J_{\rm eff} = 1/2$ magnetic Ru$^{3+}$ ions to the isotropic Heisenberg magnet CrCl$_3$ with $S = 3/2$ magnetic Cr$^{3+}$ ions. Magnetization measurements on single crystals revealed a reversal of the magnetic anisotropy under doping, which we argue to arise from the competition between anisotropic Kitaev and off-diagonal interactions on the Ru-Ru links and approximately isotropic Cr-Ru and isotropic Cr-Cr interactions. In addition, combined magnetization, ac susceptibility and specific-heat measurements clearly show the destabilization of the long-range magnetic order of $\alpha$-RuCl$_3$ in favor of a spin-glass state of Ru$_{1-x}$Cr$_x$Cl$_3$ for a low doping of $x\backsimeq0.1$. The corresponding freezing temperature as a function of Cr content shows a broad maximum around $x\backsimeq0.45$.

Highlights

  • The Kitaev model on a honeycomb lattice realizes a topological spin liquid in two space dimensions with fractionalized Majorana-fermion excitations [1,2,3]

  • Magnetic properties of the substitution series Ru1−xCrxCl3 were investigated to determine the evolution from the anisotropic Kitaev magnet α-RuCl3 with Jeff = 1/2 magnetic Ru3+ ions to the isotropic Heisenberg magnet CrCl3 with S = 3/2 magnetic Cr3+ ions

  • Magnetization measurements on single crystals revealed a reversal of the magnetic anisotropy under doping, which we argue to arise from the competition between anisotropic Kitaev and off-diagonal interactions on the Ru-Ru links and approximately isotropic Cr-Ru and isotropic Cr-Cr interactions

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Summary

INTRODUCTION

The Kitaev model on a honeycomb lattice realizes a topological spin liquid in two space dimensions with fractionalized Majorana-fermion excitations [1,2,3]. T2D = 17 K prior to the long-range antiferromagnetic ordering at 14 K was proposed from Faraday rotation and specific-heat measurements [44,45] It is the purpose of this paper to discuss the magnetic properties of the complete Ru1−xCrxCl3 series based on magnetization, specific-heat, and ac susceptibility measurements. The combination of these thermodynamic probes allows us to construct the x-T phase diagram of Ru1−xCrxCl3, where the antiferromagnetic zigzag order is replaced by a spinglass state for 0.1 x 0.7. The substitution series Ru1−xCrxCl3 constitutes one of the rare cases with simultaneous tuning of frustration and disorder

EXPERIMENTAL TECHNIQUES
Temperature dependence of the magnetization
Field dependence of the magnetization
AC MAGNETIC SUSCEPTIBILITY
HEAT CAPACITY
X-T PHASE DIAGRAM
SUMMARY AND CONCLUSION
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