Antiferromagnetic Ordering in the Frustrated Rare-Earth Chain Systems M2Cl3 (M = Gd, Tb)

IF 7.2 2区材料科学 Q2 CHEMISTRY, PHYSICAL Chemistry of Materials Pub Date : 2024-07-10 DOI:10.1021/acs.chemmater.4c01317

Reinhard K. Kremer, Walter Schnelle, Roland Eger, Arndt Simon, P. Jane Brown, Bachir Ouladdiaf, Klaus-Ulrich Neumann

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Abstract

The magnetic properties of the two isostructural rare-earth condensed octahedral-cluster chain compounds M₂Cl₃ (M = Gd, Tb) have been investigated by magnetization, heat capacity, and single-crystal neutron diffraction experiments. Both compounds exhibit antiferromagnetic order below ∼23 and ∼43 K for Gd₂Cl₃ and Tb₂Cl₃, respectively. For Gd₂Cl₃, the large negative Curie–Weiss temperature of ∼−209 K indicates substantial magnetic frustration. The magnetic moments of Gd at the two different crystallographic atom positions are aligned along the chains. Whereas at ∼14.5 K the magnetic moments at the shared edge approach the theoretically expected spin-only value of ∼7 μ_B, the moments at the geometrically frustrated apical position of the octahedra are significantly reduced. In Tb₂Cl₃, the magnetic moments lie in the plane perpendicular to the chains and are inclined with respect to each other. The Tb cations in the shared edges have a magnetic moment of 9.3 μ_B, slightly exceeding the maximum value of 9 μ_B that is expected for Tb³⁺ with J = 6 for the Russell–Saunders ground state. Neutron scattering with polarization analysis on a Tb₂Cl₃ crystal in a magnetic field reveals enhanced polarizability of the Tb moments at the frustrated apical octahedral sites.

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受挫稀土链系统 M2Cl3（M = 钆、铽）中的反铁磁有序性

通过磁化、热容量和单晶中子衍射实验，研究了两种等结构稀土凝聚八面体簇链化合物 M2Cl3（M = Gd、Tb）的磁性能。对于 Gd2Cl3 和 Tb2Cl3 而言，这两种化合物分别在 ∼23 K 和 ∼43 K 以下显示出反铁磁性秩序。对于 Gd2Cl3 而言，居里-韦斯温度为 ∼-209 K 的大负值表明存在大量磁沮度。在两个不同的晶体学原子位置上，Gd 的磁矩沿链排列。在 ∼14.5 K 时，共边的磁矩接近理论上预期的纯自旋值 ∼7 μB，而八面体几何沮度顶端位置的磁矩则显著减小。在 Tb2Cl3 中，磁矩位于垂直于链的平面上，并且相互倾斜。共边的铽阳离子的磁矩为 9.3 μB，略微超过了罗素-桑德斯基态 J = 6 的 Tb3+ 预期的最大值 9 μB。在磁场中对 Tb2Cl3 晶体进行的中子散射极化分析表明，在受挫尖顶八面体位点的 Tb 矩极化能力增强。

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来源期刊

Chemistry of Materials 工程技术-材料科学：综合

CiteScore

14.10

自引率

5.80%

发文量

929

审稿时长

1.5 months

期刊介绍： The journal Chemistry of Materials focuses on publishing original research at the intersection of materials science and chemistry. The studies published in the journal involve chemistry as a prominent component and explore topics such as the design, synthesis, characterization, processing, understanding, and application of functional or potentially functional materials. The journal covers various areas of interest, including inorganic and organic solid-state chemistry, nanomaterials, biomaterials, thin films and polymers, and composite/hybrid materials. The journal particularly seeks papers that highlight the creation or development of innovative materials with novel optical, electrical, magnetic, catalytic, or mechanical properties. It is essential that manuscripts on these topics have a primary focus on the chemistry of materials and represent a significant advancement compared to prior research. Before external reviews are sought, submitted manuscripts undergo a review process by a minimum of two editors to ensure their appropriateness for the journal and the presence of sufficient evidence of a significant advance that will be of broad interest to the materials chemistry community.