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量子自旋液体候选物钕钽酸盐（NdTaO）以及其他稀土七钽酸盐（铒钽酸盐（ErTaO）和钆钽酸盐（GdTaO））的优化通量法单晶生长

Optimized Flux Single-Crystal Growth of the Quantum Spin Liquid Candidate NdTaO and Other Rare-Earth Heptatantalates, ErTaO and GdTaO.

作者信息

Šibav Lia, Lozinšek Matic, Jagličić Zvonko, Arh Tina, Khuntia Panchanana, Zorko Andrej, Dragomir Mirela

机构信息

Jožef Stefan Institute, Jamova cesta 39, 1000 Ljubljana, Slovenia.

Jožef Stefan International Postgraduate School, Jamova cesta 39, 1000 Ljubljana, Slovenia.

出版信息

Cryst Growth Des. 2025 Jun 2;25(12):4646-4654. doi: 10.1021/acs.cgd.5c00624. eCollection 2025 Jun 18.

DOI:10.1021/acs.cgd.5c00624
PMID:40567339
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12186254/
Abstract

Single crystals are essential for characterizing a wide range of magnetic states, including exotic ones such as quantum spin liquids. This study reports a flux method for growing single crystals of NdTaO, the first quantum spin liquid candidate on a triangular spin-lattice with dominant Ising-like spin correlations. Purple NdTaO single crystals with hexagonal morphology were successfully grown by using a KMoO-BO flux. With lateral sizes up to 3.5 mm and a thickness up to 2 mm, these are the largest dimensions reported to date. The chemical composition was confirmed by powder and single-crystal X-ray diffraction along with scanning electron microscopy with energy dispersive X-ray spectroscopy. Aiming for an accurate determination of the magnetic anisotropy and its effect on the magnetic properties, NdTaO crystals were additionally analyzed by magnetic susceptibility, revealing a substantial anisotropy without long-range magnetic ordering down to 2 K. Single crystals of two novel rare-earth heptatantalates, ErTaO and GdTaO, were also grown, and their magnetic properties investigated. The magnetic anisotropy of ErTaO closely resembles that of isostructural NdTaO, indicating the possibility of a similar exotic magnetic ground state. In contrast, GdTaO shows paramagnetic behavior, consistent with previous results obtained for polycrystalline samples.

摘要

单晶对于表征广泛的磁态至关重要，包括诸如量子自旋液体等奇异磁态。本研究报告了一种生长钕钽酸盐（NdTaO）单晶的助熔剂法，NdTaO是三角自旋晶格上首个具有主导类伊辛自旋关联的量子自旋液体候选材料。通过使用KMoO-BO助熔剂成功生长出了具有六边形形态的紫色NdTaO单晶。其横向尺寸可达3.5毫米，厚度可达2毫米，这是迄今为止报道的最大尺寸。通过粉末和单晶X射线衍射以及配备能量色散X射线光谱仪的扫描电子显微镜对化学成分进行了确认。为了准确测定磁各向异性及其对磁性能的影响，还通过磁化率对NdTaO晶体进行了分析，结果表明在低至2 K时存在显著的各向异性且无长程磁有序。还生长了两种新型稀土七钽酸盐（ErTaO和GdTaO）的单晶，并对它们的磁性能进行了研究。ErTaO的磁各向异性与同结构的NdTaO非常相似，这表明可能存在类似的奇异磁基态。相比之下，GdTaO表现出顺磁行为，这与之前多晶样品的结果一致。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/97c2/12186254/b40be1762b89/cg5c00624_0011.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/97c2/12186254/d5dc30adec1a/cg5c00624_0007.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/97c2/12186254/b40be1762b89/cg5c00624_0011.jpg

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本文引用的文献

1
The Ising triangular-lattice antiferromagnet neodymium heptatantalate as a quantum spin liquid candidate.作为量子自旋液体候选材料的伊辛三角晶格反铁磁体七钽酸钕
Nat Mater. 2022 Apr;21(4):416-422. doi: 10.1038/s41563-021-01169-y. Epub 2021 Dec 30.
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Crystal structure refinement with SHELXL.使用SHELXL进行晶体结构精修。
Acta Crystallogr C Struct Chem. 2015 Jan;71(Pt 1):3-8. doi: 10.1107/S2053229614024218. Epub 2015 Jan 1.
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Materials discovery by flux crystal growth: quaternary and higher order oxides.通量晶体生长法的材料发现：四元及更高阶氧化物。
Angew Chem Int Ed Engl. 2012 Apr 16;51(16):3780-811. doi: 10.1002/anie.201102676. Epub 2012 Jan 27.