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Eu11Zn4Sn2As12: A Ferromagnetic Zintl Semiconductor with a Layered Structure Featuring Extended Zn4As6 Sheets and Ethane-like Sn2As6 Units

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    Eu11Zn4Sn2As12: A Ferromagnetic Zintl Semiconductor with a Layered Structure Featuring Extended Zn4As6 Sheets and Ethane-like Sn2As6 Units
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    • Kasey P. Devlin
      Kasey P. Devlin
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
      More by Kasey P. Devlin
    • Nasrin Kazem
      Nasrin Kazem
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
      More by Nasrin Kazem
    • Julia V. Zaikina
      Julia V. Zaikina
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
      More by Julia V. Zaikina
      Orcidhttp://orcid.org/0000-0002-8755-1926
    • Joya A. Cooley
      Joya A. Cooley
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
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    • Jackson R. Badger
      Jackson R. Badger
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
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    • James C. Fettinger
      James C. Fettinger
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
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      Orcidhttp://orcid.org/0000-0002-6428-4909
    • Valentin Taufour
      Valentin Taufour
      Department of Physics, University of California, One Shields Avenue, Davis, California 95616, United States
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    • Susan M. Kauzlarich*
      Susan M. Kauzlarich
      Department of Chemistry, University of California, One Shields Avenue, Davis, California 95616, United States
      *E-mail: [email protected]
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      Orcidhttp://orcid.org/0000-0002-3627-237X
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    Chemistry of Materials

    Cite this: Chem. Mater. 2018, 30, 20, 7067–7076
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    https://doi.org/10.1021/acs.chemmater.8b02749
    Published September 21, 2018
    Copyright © 2018 American Chemical Society
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    Abstract

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    We report the synthesis, structure, and magnetic properties of a new Zintl phase and structure type, Eu11Zn4Sn2As12. The structure and composition of this phase have been established by single-crystal X-ray diffraction and electron microprobe analysis. Eu11Zn4Sn2As12 crystallizes in monoclinic space group C2/c (No. 15) with the following lattice parameters: a = 7.5679(4) Å, b = 13.0883(6) Å, c = 31.305(2) Å, and β = 94.8444(7)° [R1 = 0.0398; wR2 = 0.0633 (all data)]. The anisotropic structural features staggered ethane-like [Sn2As6]12– units and infinite ∞2[Zn2As3]5– sheets extended in the a–b plane. Eu cations fill the space between these anionic motifs. Temperature-dependent magnetic properties and magnetoresistance of this Zintl phase have been studied, and the electronic structure and chemical bonding were elucidated using first-principles quantum chemical calculations (TB-LMTO-ASA). Quantum chemical calculations show that the ethane-like units can be considered as consisting of covalent single bonds; however, the ∞2[Zn2As3]5– sheets are best described with delocalized bonding and there is evidence of Eu–As interactions. Temperature-dependent magnetization and transport properties between 2 and 300 K show a ferromagnetic transition at 15 K, a band gap of 0.04 eV, and negative colossal magnetoresistance.

    Copyright © 2018 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.chemmater.8b02749.

    • Crystal data, structure refinement, atomic coordinates, and equivalent isotropic displacement parameters for Eu11Zn4Sn2As12; band structure diagram for Eu11Zn4Sn2As12; 2D slices and three-dimensional isosurfaces of the electron localization function (η) for Eu layers Ai and Aii; and magnetoresistance data from 120 to 300 K (PDF)

    • Crystallographic information for Eu11Zn4Sn2As12 (CIF)

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    Most electronic Supporting Information files are available without a subscription to ACS Web Editions. Such files may be downloaded by article for research use (if there is a public use license linked to the relevant article, that license may permit other uses). Permission may be obtained from ACS for other uses through requests via the RightsLink permission system: http://pubs.acs.org/page/copyright/permissions.html.

    Cited By

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    This article is cited by 15 publications.

    1. Mohd Ishtiyak, Spencer R. Watts, Bhushan Thipe, Frank Womack, Philip Adams, Xiaojian Bai, David P. Young, Svilen Bobev, Sviatoslav Baranets. Advancing Heteroanionicity in Zintl Phases: Crystal Structures, Thermoelectric and Magnetic Properties of Two Quaternary Semiconducting Arsenide Oxides, Eu8Zn2As6O and Eu14Zn5As12O. Inorganic Chemistry 2024, 63 (43) , 20226-20239. https://doi.org/10.1021/acs.inorgchem.4c01580
    2. Sviatoslav Baranets, Thimira Kandabadage, Xiaoping Wang, Xiaojian Bai, David P. Young, Svilen Bobev. Quaternary Zintl Phases Ba2InSnP3 and Ba2InSnAs3 with Complex Structures and n-Type Semiconducting Behavior. Chemistry of Materials 2024, 36 (15) , 7570-7580. https://doi.org/10.1021/acs.chemmater.4c01669
    3. Ashlee K. Hauble, Michael Y. Toriyama, Stephan Bartling, Ali M. Abdel-Mageed, G. Jeffrey Snyder, Susan M. Kauzlarich. Experiment and Theory in Concert To Unravel the Remarkable Electronic Properties of Na-Doped Eu11Zn4Sn2As12: A Layered Zintl Phase. Chemistry of Materials 2023, 35 (18) , 7719-7729. https://doi.org/10.1021/acs.chemmater.3c01509
    4. Siméon Ponou, Sven Lidin, Anja-Verena Mudring. Optimization of Chemical Bonding through Defect Formation and Ordering─The Case of Mg7Pt4Ge4. Inorganic Chemistry 2023, 62 (22) , 8519-8529. https://doi.org/10.1021/acs.inorgchem.2c04312
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    6. Kasey P. Devlin, Junjie Zhang, James C. Fettinger, Eun Sang Choi, Ashlee K. Hauble, Valentin Taufour, Raphael P. Hermann, Susan M. Kauzlarich. Deconvoluting the Magnetic Structure of the Commensurately Modulated Quinary Zintl Phase Eu11–xSrxZn4Sn2As12. Inorganic Chemistry 2021, 60 (8) , 5711-5723. https://doi.org/10.1021/acs.inorgchem.0c03769
    7. Zhiyu Zhou, Ziwen Wang, Xiyu Chen, Jia-Yi Lu, Junchao Zhang, Xiong Luo, Guang-Han Cao, Shuai Dong, Zhi-Cheng Wang. Unusual magnetic and transport properties in the Zintl phase Eu 11 Zn 6 As 12 . Physical Review Materials 2024, 8 (11) https://doi.org/10.1103/PhysRevMaterials.8.114421
    8. Yongqi Yang, Guangming Cheng, Joanna Blawat, Duncan H. Moseley, Haozhe Wang, Kasey P. Devlin, Yu Yu, Raphaël P. Hermann, Nan Yao, Rongying Jin, Weiwei Xie. Crystal structure and magnetic properties in semiconducting Eu3−δZn x Sn y As3 with Eu-Eu dimers. Journal of Applied Physics 2022, 132 (4) https://doi.org/10.1063/5.0094013
    9. J. C. Souza, S. M. Thomas, E. D. Bauer, J. D. Thompson, F. Ronning, P. G. Pagliuso, P. F. S. Rosa. Microscopic probe of magnetic polarons in antiferromagnetic Eu 5 In 2 Sb 6 . Physical Review B 2022, 105 (3) https://doi.org/10.1103/PhysRevB.105.035135
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    15. Alexander Ovchinnikov, Gregory M. Darone, Bayrammurad Saparov, Svilen Bobev. Exploratory Work in the Quaternary System of Ca–Eu–Cd–Sb: Synthesis, Crystal, and Electronic Structures of New Zintl Solid Solutions. Materials 2018, 11 (11) , 2146. https://doi.org/10.3390/ma11112146
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    Chemistry of Materials

    Cite this: Chem. Mater. 2018, 30, 20, 7067–7076
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.chemmater.8b02749
    Published September 21, 2018
    Copyright © 2018 American Chemical Society
    Request reuse permissions

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