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对 (Eu(1-x)Ca(x))9In8(Ge(1-y)Sn(y))8（x = 0.66，y = 0.03）和 (Eu(1-x)Ca(x))3In(Ge(3-y)Sn(1+y))（x = 0.66，0.68；y = 0.13，0.27）相中的三种五元极性金属间化合物的晶体结构、化学键和磁性研究

Crystal structure, chemical bonding and magnetism studies for three quinary polar intermetallic compounds in the (Eu(1-x)Ca(x))9In8(Ge(1-y)Sn(y))8 (x = 0.66, y = 0.03) and the (Eu(1-x)Ca(x))3In(Ge(3-y)Sn(1+y)) (x = 0.66, 0.68; y = 0.13, 0.27) phases.

作者信息

Woo Hyein, Jang Eunyoung, Kim Jin, Lee Yunho, Kim Jongsik, You Tae-Soo

机构信息

Department of Chemistry, Chungbuk National University, Cheongju, Chungbuk 362-763, Korea.

Department of Chemistry, Korea Advanced Institute of Science and Technology, Daejeon 305-701, Korea.

出版信息

Int J Mol Sci. 2015 Apr 22;16(4):9017-36. doi: 10.3390/ijms16049017.

DOI:10.3390/ijms16049017
PMID:25913380
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC4425121/
Abstract

Three quinary polar intermetallic compounds in the (Eu(1-x)Ca(x))9In8(Ge(1-y)Sn(y))8 (x = 0.66, y = 0.03) and the (Eu(1-x)Ca(x))3In(Ge(3-y)Sn(1+y)) (x = 0.66, 0.68; y = 0.13, 0.27) phases have been synthesized using the molten In-metal flux method, and the crystal structures are characterized by powder and single-crystal X-ray diffractions. Two orthorhombic structural types can be viewed as an assembly of polyanionic frameworks consisting of the In(Ge/Sn)4 tetrahedral chains, the bridging Ge2 dimers, either the annulene-like "12-membered rings" for the (Eu(1-x)Ca(x))9In8(Ge(1-y)Sn(y))8 series or the cis-trans Ge/Sn-chains for the (Eu(1-x)Ca(x))3In(Ge(3-y)Sn(1+y)) series, and several Eu/Ca-mixed cations. The most noticeable difference between two structural types is the amount and the location of the Sn-substitution for Ge: only a partial substitution (11%) occurs at the In(Ge/Sn)4 tetrahedron in the (Eu(1-x)Ca(x))9In8(Ge(1-y)Sn(y))8 series, whereas both a complete and a partial substitution (up to 27%) are observed, respectively, at the cis-trans Ge/Sn-chain and at the In(Ge/Sn)4 tetrahedron in the (Eu(1-x)Ca(x))3In(Ge(3-y)Sn(1+y)) series. A series of tight-binding linear muffin-tin orbital calculations is conducted to understand overall electronic structures and chemical bonding among components. Magnetic susceptibility measurement indicates a ferromagnetic ordering of Eu atoms below 5 K for Eu1.02(1)Ca1.98InGe2.87(1)Sn1.13.

摘要

采用金属铟熔盐法合成了(Eu(1 - x)Ca(x))9In8(Ge(1 - y)Sn(y))8（x = 0.66，y = 0.03）和(Eu(1 - x)Ca(x))3In(Ge(3 - y)Sn(1 + y))（x = 0.66，0.68；y = 0.13，0.27）相中的三种五元极性金属间化合物，并通过粉末和单晶X射线衍射对其晶体结构进行了表征。两种正交结构类型可视为由In(Ge/Sn)4四面体链、桥连的Ge2二聚体、(Eu(1 - x)Ca(x))9In8(Ge(1 - y)Sn(y))8系列中的类苯“12元环”或(Eu(1 - x)Ca(x))3In(Ge(3 - y)Sn(1 + y))系列中的顺反Ge/Sn链以及几种Eu/Ca混合阳离子组成的聚阴离子框架的组装体。两种结构类型之间最显著的差异在于Ge被Sn取代的量和位置：在(Eu(1 - x)Ca(x))9In8(Ge(1 - y)Sn(y))8系列中，仅在In(Ge/Sn)4四面体上发生部分取代（11%），而在(Eu(1 - x)Ca(x))3In(Ge(3 - y)Sn(1 + y))系列中，分别在顺反Ge/Sn链和In(Ge/Sn)4四面体上观察到完全取代和部分取代（高达27%）。进行了一系列紧束缚线性 muffin-tin轨道计算，以了解各组分之间的整体电子结构和化学键。磁化率测量表明，对于Eu1.02(1)Ca1.98InGe2.87(1)Sn1.13，Eu原子在5 K以下呈现铁磁有序。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/92743368429c/ijms-16-09017-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/e171cd5aa815/ijms-16-09017-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/f3e67f27aff8/ijms-16-09017-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/5201cfb82e50/ijms-16-09017-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/46e2bb1dabd0/ijms-16-09017-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/ef19297c3a38/ijms-16-09017-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/f01b68b87d1a/ijms-16-09017-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/92743368429c/ijms-16-09017-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/e171cd5aa815/ijms-16-09017-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/f3e67f27aff8/ijms-16-09017-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/5201cfb82e50/ijms-16-09017-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/46e2bb1dabd0/ijms-16-09017-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/ef19297c3a38/ijms-16-09017-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/f01b68b87d1a/ijms-16-09017-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/4700/4425121/92743368429c/ijms-16-09017-g007.jpg

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