论文标题

量子旋转液体中的晶体电场激发候选$ naybse_ {2} $

Crystalline Electric-Field Excitations in Quantum Spin Liquids Candidate $NaYbSe_{2}$

论文作者

Zhang, Zheng, Ma, Xiaoli, Li, Jianshu, Wang, Guohua, Adroja, D. T., Perring, T. G., Liu, Weiwei, Jin, Feng, Ji, Jianting, Wang, Yimeng, Wang, Xiaoqun, Ma, Jie, Zhang, Qingming

论文摘要

最近,我们透露了一大批三角形晶格量子自旋液体候选物,称为稀土红ogogenides,该液体具有高对称结构,而没有结构/电荷障碍和自旋杂质,并且可以用作探索自旋液体物理学的理想平台。晶体电场(CEF)激发的知识是探索稀土自旋系统的基本磁性的重要步骤。在这里,我们采用了非弹性中子散射(INS)和拉曼散射(RS),对$ naybse_ {2} $的全面调查,是该家庭的有前途的代表。与其非磁化合物$ naluse_ {2} $相比,我们能够在5k时以15.8、24.3和30.5 MEV识别CEF激发。 INS光谱的选定剪辑通过$ g $因子的大型各向异性($ g_ {ab}:g_ {c} \ sim3:1 $)进行了很好的重新生产。此外,根据点电荷模型,我们的计算很好地解释了CEF激发。有趣的是,$ naybse_ {2} $随着温度升高而表现出异常的CEF转移到更高的能量,而接近第一个CEF激发的拉曼模式显示出随着温度降低的较大较大的软化。 $ naluse_ {2} $中的异常缺失清楚地表明了家庭中未报告的cef-phonon耦合。可以从SE的较弱的电负性术语中理解。 $ naybch_ {2} $的子家庭中最小的第一架CEF激发是$ \ sim $ 180K(ch = o,s,se),保证可以在足够低的温度下用有效的S = 1/2图片来严格描述子家庭。有趣的是,此处揭示的CEF-Phonon耦合可能会提出操纵自旋系统的其他可能性。

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 $NaYbSe_{2}$, a promising representative of the family. By comparison with its nonmagnetic compound $NaLuSe_{2}$, 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 ($g_{ab}:g_{c}\sim3:1$). Further, the CEF excitations are explained well by our calculations based on the point charge model. Interestingly, $NaYbSe_{2}$ 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 $NaLuSe_{2}$ 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 $NaYbCh_{2}$ 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.

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