Abstract

Recently, several putative quantum spin liquid (QSL) states were discovered in {\tilde S} = 1/2S̃=1/2 rare-earth based triangular-lattice antiferromagnets (TLAF) with the delafossite structure. In order to elucidate the conditions for a QSL to arise, we report here the discovery of a long-range magnetic order in the Ce-based TLAF KCeS_22 below T_{\mathrm N} = 0.38TN=0.38 K, despite the same delafossite structure. Finally, combining various experimental and computational methods, we characterize the crystal electric field scheme, the magnetic anisotropy and the magnetic ground state of KCeS_22.

Highlights

  • Magnetic frustration is at interest because it can lead to the competition of a large variety of emergent states of broken magnetic symmetry and the possible realization of quantum spin liquid (QSL) states [1,2,3]

  • At the base temperature T = 5 K, the width of the crystal electric field (CEF) lines is limited by the experimental energy resolution, evidencing the absence of any considerable CEF randomness resulting from the site intermixing that was reported, for instance, in YbMgGaO4 [55]

  • Specific heat measurements of each of these QSL candidates indicate a broad maximum of Cp/T around the temperature corresponding to the possible formation of the spin liquid state [19,22,27,29,30]

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Summary

Introduction

Magnetic frustration is at interest because it can lead to the competition of a large variety of emergent states of broken magnetic symmetry and the possible realization of quantum spin liquid (QSL) states [1,2,3]. In particular materials with a QSL ground state have caused an abiding fascination within the scientific community due to its strong quantum entanglement, while long-range magnetic order is absent down to zero temperature This exotic spin-disordered state displays fractionalized quasiparticle excitations relevant for topological quantum computation [4]. A second nearest-neighbor interaction J2 can destabilize the 120◦ spin-ordered phase into a quantum spin liquid state as shown by DMRG [9, 10] and variational Monte Carlo calculations [11]. Second nearest-neighbor interactions were proposed as a possible origin of the QSL state [33] and at this time the source of the quantum spin liquid state in the rare-earth based TLAFs remains still under debate [3]. This reveals an in-plane anisotropy, which may indicate anisotropic magnetic interactions in KCeS2

Crystal growth and structural analyses
Experimental and computational techniques
Magnetization measurements
ESR measurements
Inelastic neutron scattering
Quantum chemical calculations
Specific heat measurements
Magne tic Order
Findings
10 Discussion
11 Conclusion
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