手性三元硫属化合物Eu2SiSe4的磁性和大二次谐波产生响应

IF 7 2区 材料科学 Q2 CHEMISTRY, PHYSICAL
Shaun O’Donnell, Ian A. Leahy, Subhendu Jana, Eric A. Gabilondo, P. Shiv Halasyamani, Paul A. Maggard, Rebecca W. Smaha
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引用次数: 0

摘要

含Eu(II)硫族化合物是一类新兴的材料,由于其高光活性和迷人的磁性而引起了人们的极大兴趣。在此,我们合成了Eu2SiSe4为红色单晶,并用单晶x射线衍射对其结构进行了表征,在室温下证实了所报道的手性单斜P21对称性。Eu2SiSe4的晶体结构由扭曲的SiSe4四面体单元和电荷平衡的Eu(II)阳离子组成。在这里,我们开发了一种两步固态合成Eu2SiSe4的方法,并将其与已知的硫族化硼方法进行了比较。我们发现多晶Eu2SiSe4的二次谐波生成(SHG)活性为~ 7 × AgGaS2,使其成为已知的SHG活性最高的硫族化合物之一。在单晶x射线衍射中,在100 K以下没有观察到对称性降低,尽管b轴晶格参数出现了异常扩展,并且可能与SiSe4四面体的晶格模式有关。我们利用磁强计和热容测量研究了Eu2SiSe4的物理性质,并发现在TN≈5.5 K时跃迁到反铁磁基态。低温转变释放的熵比预期的要少,这可能是由于Eu(II)复杂的晶体电场效应。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Magnetic Properties and Large Second-Harmonic Generation Response of a Chiral Ternary Chalcogenide: Eu2SiSe4
Eu(II)-containing chalcogenides are an emerging class of materials that are of great interest due to their high optical activity and intriguing magnetism. Here, we synthesized Eu2SiSe4 as red-colored single crystals and characterized its structure with single-crystal X-ray diffraction, confirming the reported chiral monoclinic P21 symmetry at room temperature. The crystal structure of Eu2SiSe4 comprises distorted SiSe4 tetrahedral units and charge-balancing Eu(II) cations. Here, we develop a two-step solid-state synthesis method for Eu2SiSe4 and compare it to the known boron chalcogenide method. We find the second-harmonic generation (SHG) activity of polycrystalline Eu2SiSe4 to be ∼7 × AgGaS2, placing it among the highest-known SHG-active chalcogenides. No symmetry lowering is observed down to 100 K in single-crystal X-ray diffraction, although an anomalous expansion in the b-axis lattice parameter occurs and may be correlated to lattice modes of the SiSe4 tetrahedra. We investigate the physical properties of Eu2SiSe4 using magnetometry and heat capacity measurements and find a transition to an antiferromagnetic ground state at TN ≈ 5.5 K. The low-temperature transition releases less entropy than expected, which may be due to the complex crystal electric field effects of Eu(II).
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来源期刊
Chemistry of Materials
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.
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