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中国物理学会期刊

稀土基三角阻挫金属间化合物LnNiAl4Ge2(Ln=Gd,Tb,Dy,Ho,Er)的单晶生长及磁相变

Single Crystal Growth and Magnetic Phase Transitions of Rare-Earth-Based Triangular Lattice Frustrated Intermetallic Compounds LnNiAl4Ge2 (Ln = Gd, Tb, Dy, Ho, Er)

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  • 稀土基三角晶格金属间化合物因其内部几何阻挫、晶体场效应与Ruderman-Kittel-Kasuya-Yosida (RKKY)交换作用的结合能产生复杂而有趣的物理现象,在材料科学和凝聚态物理中引起了极大的关注。本文采用Al-Ge自助熔剂法成功生长出一系列高质量稀土基三角晶格金属间化合物LnNiAl4Ge2(Ln=Gd,Tb,Dy,Ho,Er)单晶,并系统地研究了他们的晶体结构及磁性,其中TbNiAl4Ge2、HoNiAl4Ge2和ErNiAl4Ge2的单晶磁性为首次报道。单晶和粉末X射线衍射分析表明,所有化合物均结晶于三方晶系的R3m空间群,稀土磁性离子在ab面内构成三角晶格。磁化率及比热测试显示,从Gd到Ho,磁相变温度随稀土离子半径减小而单调降低,Er的磁有序温度可能低于2 K,整体变化趋势与de Gennes因子的变化趋势基本一致,表明RKKY交换作用在磁相互作用中占主导地位。此外,2 K下的等温磁化曲线揭示了这些材料具有不同的磁各向异性: GdNiAl4Ge2具有各向同性,TbNiAl4Ge2为强易面各向异性,DyNiAl4Ge2和HoNiAl4Ge2呈现XXZ型各向异性,ErNiAl4Ge2则为易轴各向异性,这表明晶体场效应对磁各向异性有显著调制作用。本研究为理解稀土金属三角晶格体系中几何阻挫、RKKY相互作用与晶体场效应之间的关联提供了系统的实验数据。

    The interplay of geometric frustration, crystal electric field effects, and Ruderman-Kittel-Kasuya-Yosida (RKKY) exchange interaction can give rise to complex and intriguing magnetic behaviors in rare-earth-based triangular lattice intermetallic compounds. In this work, high-quality single crystals of LnNiAl4Ge2 (Ln = Gd, Tb, Dy, Ho, Er) were successfully grown using the Al-Ge self-flux method, and their crystal structures, magnetic properties, and specific heat were systematically investigated. X-ray diffraction analysis shows that all compounds crystallize in the centrosymmetric rhombohedral structure with space group R¯ 3m, where the rare-earth ions form a two-dimensional triangular lattice within the ab plane. Magnetic susceptibility and specific heat measurements reveal that GdNiAl4Ge2 undergoes two successive transitions at 15.35 K and 8.77 K, TbNiAl4Ge2 has a single transition at 8.83 K, DyNiAl4Ge2 at 8.07 K, HoNiAl4Ge2 at 5.83 K and 4.29 K, whereas ErNiAl4Ge2 shows no magnetic order above 2 K. From Gd to Ho, the magnetic transition temperatures decrease systematically with decreasing rare-earth ionic radius, while for Er the magnetic ordering temperature is likely below 2 K, and the overall trend is in agreement with that of the de Gennes factor, indicating the dominant role of the RKKY exchange interaction in the magnetic behavior. The isothermal magnetization curves measured at 2 K reveal that GdNiAl4Ge2 is nearly isotropic with a subtle hysteresis loop near 0.42 T, while the other compounds exhibit distinct magnetic anisotropies due to crystal electric field effects: TbNiAl4Ge2 shows strong easyplane anisotropy, DyNiAl4Ge2 and HoNiAl4Ge2 display complex XXZ-type anisotropy, and ErNiAl4Ge2 exhibits easy-axis anisotropy. Furthermore, rich field-induced metamagnetic transitions are observed: TbNiAl4Ge2 shows two transitions in the ab plane at 0.40 T and 2.00 T; DyNiAl4Ge2 exhibits two transitions in the ab plane at 0.65 T and 1.25 T and two along the c axis at 0.62 T and 3.92 T; HoNiAl4Ge2 displays two transitions in the ab plane at 0.35 T and 0.55 T and one along the c axis at 0.34 T; ErNiAl4Ge2 shows a single transition in the ab plane near 9.25 T and an anomalous high-field feature along the c axis likely related to spin reorientation. Additionally, broad CEF-derived peaks appear around 85 K along the c axis for TbNiAl4Ge2 and around 30 K in the ab plane for ErNiAl4Ge2. The single-crystal magnetic properties of TbNiAl4Ge2, HoNiAl4Ge2, and ErNiAl4Ge2 are reported here for the first time. This study provides systematic experimental results for further studies to understand the interplay among geometric frustration, RKKY interaction, and crystal electric field effects in metallic triangular lattice systems.

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