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Intricate Short-Range Ordering and Strongly Anisotropic Transport Properties of Li1–x Sn 2+x As2

Journal Article · · Journal of the American Chemical Society
DOI:https://doi.org/10.1021/jacs.5b00237· OSTI ID:1334418
 [1];  [2];  [2];  [3];  [3];  [4];  [4];  [5];  [5];  [6];  [1]
  1. Univ. of California, Davis, CA (United States). Dept. of Chemistry
  2. Univ. of California, Davis, CA (United States). Dept. of of Chemical Engineering and Materials Science
  3. Florida State Univ., Tallahassee, FL (United States). Center of Interdisciplinary Magnetic Resonance, National High Magnetic Field Lab. (MagLab)
  4. Univ. of Munster, Munster (Germany). Inst. of Inorganic and Analytical Chemistry
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical and Engineering Materials Division
  6. Univ. of Caen, Caen (France). CRISMAT Lab.
+ Show Author Affiliations
A new ternary compound, Li1-xSn2+xAs2, 0.2 < x < 0.4, was synthesized via solid-state reaction of elements. The compound crystallizes in a layered structure in the R$$\overline{3}m$$ space group (No. 166) with Sn-As layers separated by layers of jointly occupied Li/Sn. The Sn-As layers are comprised of Sn3As3 puckered hexagons in a chair conformation that share all edges. Li/Sn atoms in the interlayer space are surrounded by a regular As6 octahedron. Thorough investigations by synchrotron x-ray and neutron powder diffraction indicate no long-range Li/Sn ordering. In contrast, local Sn/Li ordering was revealed by synergistic investigations via solid-state 6,7Li NMR spectroscopy, HR-TEM, and neutron and X-ray pair distribution function analyses. Due to their different chemical natures, Li and Sn atoms tend to segregate into Li-rich and Sn-rich regions creating substantial inhomogeneity on the nanoscale. Inhomogeneous local structure has high impact on the physical properties of the synthesized compounds: local Li/Sn ordering and multiple nanoscale interfaces result in unexpectedly low thermal conductivity and highly anisotropic resistivity in Li1-xSn2+xAs2.
Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Grant/Contract Number:
AC05-00OR22725; SC0008931; AC02-06CH11357
OSTI ID:
1334418
Alternate ID(s):
OSTI ID: 1176800
Journal Information:
Journal of the American Chemical Society, Journal Name: Journal of the American Chemical Society Journal Issue: 10 Vol. 137; ISSN 0002-7863
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

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Crystal and Electronic Structure and Optical Properties of AE 2 SiP 4 ( AE = Sr, Eu, Ba) and Ba 4 Si 3 P 8 : Crystal and Electronic Structure and Optical Properties of journal November 2018
Two-dimensional metal NaCu 6.3 Sb 3 and solid-state transformations of sodium copper antimonides journal January 2017
Synthesis, structure, and transport properties of Ba 8 Cu 16 –  x Au x P 30 clathrate solid solution journal February 2020
Temperature dependent local atomic displacements in NaSn 2 As 2 system journal July 2019

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