Crystalline Electric-Field Excitations in Quantum Spin Liquids Candidate $NaYbS{e}_2$

Abstract

Very recently we revealed a large family of triangular lattice quantum spin liquid candidates named rare-earth chalcogenides, which features a high-symmetry structure without structural/charge disorders and spin impurities, and may serve as an ideal platform exploring spin liquid physics. The knowledge of crystalline electric-field (CEF) excitations is an essential step to explore the fundamental magnetism of rare-earth spin systems. Here we employed inelastic neutron scattering (INS) and Raman scattering (RS) to carry out a comprehensive CFE investigation on $NaYbS{e}_2$, a promising representative of the family. By comparison with its nonmagnetic compound $NaLuS{e}_2$, we are able to identify the CEF excitations at 15.8, 24.3 and 30.5 meV at 5K. The selected cuts of the INS spectra are well re-produced with a large anisotropy of $g$ factors ($g_{ab}:g_c\sim 3:1$). Further, the CEF excitations are explained well by our calculations based on the point charge model. Interestingly, $NaYbS{e}_2$ exhibits an unusual CEF shift to higher energies with increasing temperatures, and the Raman mode close to the first CEF excitation shows an anomalously large softening with decreasing temperatures. The absence of the anomalies in $NaLuS{e}_2$ clearly demonstrates a CEF-phonon coupling not reported in the family. It can be understood in term of the weaker electronegativity of Se. The fact that the smallest first CEF excitation in the sub-family of $NaYbC{h}_2$ is $\sim$ 180K (Ch=O, S, Se), guarantees that the sub-family can be strictly described with an effective S=1/2 picture at sufficiently low temperatures. Interestingly the CEF-phonon coupling revealed here may present alternative possibilities to manipulate the spin systems.

7 pages, 4 figures, supplementary material provided, error corrected in Figure 4

References in corpus (23)

• Anyons in an exactly solved model and beyond
• Quantum Spin Liquids
• Mantid - Data Analysis and Visualization Package for Neutron Scattering and $\mu SR$ Experiments
• Fractionalized excitations in the spin liquid state of a kagomé lattice antiferromagnet
• Rare-earth triangular lattice spin liquid: a single-crystal study of YbMgGaO${}_4$
• Evidence for a spinon Fermi surface in a triangular lattice quantum spin liquid candidate
• Gapless quantum spin liquid ground state in the two-dimensional spin-1/2 triangular antiferromagnet YbMgGaO${}_4$
• Field-tunable quantum disordered ground state in the triangular lattice antiferromagnet NaYbO${}_2$
• $\mu$SR evidence for the U(1) quantum spin liquid ground state in the triangular antiferromagnet YbMgGaO${}_4$
• Rare-earth chalcogenides: A large family of triangular lattice spin liquid candidate
• Crystalline Electric Field Randomness in the Triangular Lattice Spin-Liquid YbMgGaO${}_4$
• NaYbS${}_2$ - a new planar spin-$\frac{1}{2}$ triangular-lattice magnet and putative spin liquid
• Gapless spin-liquid state in the structurally disorder-free triangular antiferromagnet NaYbO${}_2$
• Anisotropic field-induced ordering in the triangular-lattice quantum spin liquid NaYbSe${}_2$
• Field-induced instability of the quantum-spin-liquid ground state in the $J_{\mathrm{eff}}=\frac{1}{2}$ triangular-lattice compound NaYbO${}_2$
• Field-induced magnetic transition and spin fluctuation in quantum spin liquid candidate CsYbSe${}_2$
• A Class of Compounds Featuring Frustrated Triangular Magnetic Lattice CsRESe${}_2$ (RE=La-Lu): Quantum Spin-Liquid Candidates
• Nearest-neighbor resonating valence bonds in YbMgGaO4
• Crystal field parameters of the rare earth pyrochlores $R_2$Ti${}_2$O${}_7$ ($R$ = Tb, Dy, Ho)
• Synthesis, magnetization and heat capacity of triangular lattice materials NaErSe${}_2$ and KErSe${}_2$
• Single-site magnetic anisotropy governed by inter-layer cation charge imbalance in triangular-lattice AYbX${}_2$
• Emergent Vibronic Excitations in the Magnetodielectric Regime of ${\text{Ce}}_2{\text{O}}_3$: Raman Scattering Studies
• Crystal-electric-field excitations in a quantum-spin-liquid candidate NaErS${}_2$

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