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Title: Unique [Mn6Bi5]- Nanowires in KMn6Bi5: A Quasi-One-Dimensional Antiferromagnetic Metal

Abstract

In this paper, we report a new quasi-one-dimensional compound KMn6Bi5 composed of parallel nanowires crystallizing in a monoclinic space group C2/m with a = 22.994(2) Å, b = 4.6128(3) Å, c = 13.3830(13) Å and β = 124.578(6)°. The nanowires are infinite [Mn6Bi5]- columns each of which is composed of a nanotube of Bi atoms acting as the cladding with a nanorod of Mn atoms located in the central axis of the nanotubes. The nanorods of Mn atoms inside the Bi cladding are stabilized by Mn–Mn bonding and are defined by distorted Mn-centered cluster icosahedra of Mn13 sharing their vertices along the b axis. The [Mn6Bi5]- nanowires are linked with weak internanowire Bi–Bi bonds and charge balanced with K+ ions. The [Mn6Bi5]- nanowires were directly imaged by high-resolution transmission electron microscopy and scanning transmission electron microscopy. Magnetic susceptibility studies show one-dimensional characteristics with an antiferromagnetic transition at ~75 K and a small average effective magnetic moment (1.56 μB/Mn for H ∥ b and 1.37 μB/Mn for H ⊥ b) of Mn from Curie–Weiss fits above 150 K. Specific heat measurements reveal an electronic specific heat coefficient γ of 6.5(2) mJ K–2(mol-Mn)-1 and a small magnetic entropy change ΔSmag ≈ 1.6more » J K–1 (mol-Mn)-1 across the antiferromagnetic transition. Finally, in contrast to a metallic resistivity along the column, the resistivity perpendicular to the column shows a change from a semiconducting behavior at high temperatures to a metallic one at low temperatures, indicating an incoherent-to-coherent crossover of the intercolumn tunneling of electrons.« less

Authors:
ORCiD logo [1];  [2];  [3];  [4];  [2];  [5];  [5];  [6];  [2]; ORCiD logo [7]; ORCiD logo [8]; ORCiD logo [3]; ORCiD logo [6]; ORCiD logo [9]
  1. Zhejiang Univ., Hangzhou (China). Dept. of Physics; Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  2. Zhejiang Univ., Hangzhou (China). Dept. of Physics
  3. Northwestern Univ., Evanston, IL (United States). Dept. of Materials Science and Engineering
  4. Zhejiang Univ., Hangzhou (China). Dept. of Chemistry
  5. Hangzhou Normal Univ. (China). Dept. of Physics
  6. Zhejiang Univ., Hangzhou (China). Dept. of Physics. State Key Lab. of Silicon Materials; Nanjing Univ. (China). Collaborative Innovation Centre of Advanced Microstructures
  7. Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
  8. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  9. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Northwestern Univ., Evanston, IL (United States). Dept. of Chemistry
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Northwestern Univ., Evanston, IL (United States); Zhejiang Univ., Hangzhou (China)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF); National Natural Science Foundation of China (NNSFC); National Key Research and Development Program of China
OSTI Identifier:
1433916
Grant/Contract Number:  
AC02-06CH11357; ECCS-1542205; DMR-1720139; 11674281; 2017YFA0303002
Resource Type:
Accepted Manuscript
Journal Name:
Journal of the American Chemical Society
Additional Journal Information:
Journal Volume: 140; Journal Issue: 12; Journal ID: ISSN 0002-7863
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; 71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSICS

Citation Formats

Bao, Jin-Ke, Tang, Zhang-Tu, Jung, Hee Joon, Liu, Ji-Yong, Liu, Yi, Li, Lin, Li, Yu-Ke, Xu, Zhu-An, Feng, Chun-Mu, Chen, Haijie, Chung, Duck Young, Dravid, Vinayak P., Cao, Guang-Han, and Kanatzidis, Mercouri G.. Unique [Mn6Bi5]- Nanowires in KMn6Bi5: A Quasi-One-Dimensional Antiferromagnetic Metal. United States: N. p., 2018. Web. https://doi.org/10.1021/jacs.8b00465.
Bao, Jin-Ke, Tang, Zhang-Tu, Jung, Hee Joon, Liu, Ji-Yong, Liu, Yi, Li, Lin, Li, Yu-Ke, Xu, Zhu-An, Feng, Chun-Mu, Chen, Haijie, Chung, Duck Young, Dravid, Vinayak P., Cao, Guang-Han, & Kanatzidis, Mercouri G.. Unique [Mn6Bi5]- Nanowires in KMn6Bi5: A Quasi-One-Dimensional Antiferromagnetic Metal. United States. https://doi.org/10.1021/jacs.8b00465
Bao, Jin-Ke, Tang, Zhang-Tu, Jung, Hee Joon, Liu, Ji-Yong, Liu, Yi, Li, Lin, Li, Yu-Ke, Xu, Zhu-An, Feng, Chun-Mu, Chen, Haijie, Chung, Duck Young, Dravid, Vinayak P., Cao, Guang-Han, and Kanatzidis, Mercouri G.. Thu . "Unique [Mn6Bi5]- Nanowires in KMn6Bi5: A Quasi-One-Dimensional Antiferromagnetic Metal". United States. https://doi.org/10.1021/jacs.8b00465. https://www.osti.gov/servlets/purl/1433916.
@article{osti_1433916,
title = {Unique [Mn6Bi5]- Nanowires in KMn6Bi5: A Quasi-One-Dimensional Antiferromagnetic Metal},
author = {Bao, Jin-Ke and Tang, Zhang-Tu and Jung, Hee Joon and Liu, Ji-Yong and Liu, Yi and Li, Lin and Li, Yu-Ke and Xu, Zhu-An and Feng, Chun-Mu and Chen, Haijie and Chung, Duck Young and Dravid, Vinayak P. and Cao, Guang-Han and Kanatzidis, Mercouri G.},
abstractNote = {In this paper, we report a new quasi-one-dimensional compound KMn6Bi5 composed of parallel nanowires crystallizing in a monoclinic space group C2/m with a = 22.994(2) Å, b = 4.6128(3) Å, c = 13.3830(13) Å and β = 124.578(6)°. The nanowires are infinite [Mn6Bi5]- columns each of which is composed of a nanotube of Bi atoms acting as the cladding with a nanorod of Mn atoms located in the central axis of the nanotubes. The nanorods of Mn atoms inside the Bi cladding are stabilized by Mn–Mn bonding and are defined by distorted Mn-centered cluster icosahedra of Mn13 sharing their vertices along the b axis. The [Mn6Bi5]- nanowires are linked with weak internanowire Bi–Bi bonds and charge balanced with K+ ions. The [Mn6Bi5]- nanowires were directly imaged by high-resolution transmission electron microscopy and scanning transmission electron microscopy. Magnetic susceptibility studies show one-dimensional characteristics with an antiferromagnetic transition at ~75 K and a small average effective magnetic moment (1.56 μB/Mn for H ∥ b and 1.37 μB/Mn for H ⊥ b) of Mn from Curie–Weiss fits above 150 K. Specific heat measurements reveal an electronic specific heat coefficient γ of 6.5(2) mJ K–2(mol-Mn)-1 and a small magnetic entropy change ΔSmag ≈ 1.6 J K–1 (mol-Mn)-1 across the antiferromagnetic transition. Finally, in contrast to a metallic resistivity along the column, the resistivity perpendicular to the column shows a change from a semiconducting behavior at high temperatures to a metallic one at low temperatures, indicating an incoherent-to-coherent crossover of the intercolumn tunneling of electrons.},
doi = {10.1021/jacs.8b00465},
journal = {Journal of the American Chemical Society},
number = 12,
volume = 140,
place = {United States},
year = {2018},
month = {3}
}

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