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Title: Indium Preferential Distribution Enables Electronic Engineering of Magnetism in FeSb2–xInxSe4 p-Type High-Tc Ferromagnetic Semiconductors

Journal Article · · Chemistry of Materials
 [1];  [1];  [1];  [2];  [1];  [1];  [1];  [1];  [1];  [1]
  1. Univ. of Michigan, Ann Arbor, MI (United States)
  2. Univ. of Michigan, Ann Arbor, MI (United States); Governors State Univ., University Park, IL (United States)
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In this work, single-phase samples of the solid-solution series FeSb2–xInxSe4 (0 ≤ x ≤ 0.25) were synthesized using solid-state reaction of the elements to probe the effect of electronic structure engineering on the magnetic behavior of the p-type semiconductor, FeSb2Se4. Powder X-ray diffraction data suggest that all samples are isostructural with FeSb2Se4. Rietveld refinements of the distribution of In atoms at various metal positions indicate a preferential substitution of Sb at the M1(4i) position within the magnetic layer A for In concentration up to x = 0.1. FeSb2–xInxSe4 compositions with higher In content show the distribution of In atoms at all metal positions, except for the M3(2d), which is fully occupied by Fe atoms. Interestingly, the ordering of Fe atoms within the crystal structure of FeSb2–xInxSe4 remains essentially unaffected by the degree of substitution (x values) and is comparable to the distribution of Fe atoms reported in FeSb2Se4. X-ray photoelectron spectroscopy confirms the oxidation states of various metal atoms In(+3), Sb(+3), Fe(+2) in the structure. Electronic transport properties indicate p-type semiconducting behavior for all samples. The electrical conductivity above 300 K first increases with In content, reaches the maximum value for x = 0.1, then decreases with further increase in In content. A reverse trend is observed for the thermopower. All samples show drastically low thermal conductivity with room temperature values ranging from 0.45 Wm–1 K–1 for x = 0 to 0.27 Wm–1 K–1 for the sample with x = 0.25. Magnetic susceptibility data suggest ferromagnetic-like behavior from 2–300 K for all samples. The magnitude of the magnetic susceptibility rapidly increases with In content, reaches a maximum for x = 0.1, and marginally decreases with further increase in In concentration. The observed surprising change in the magnetic and electronic behavior of samples with high In content (x > 0.1) is rationalized using the concept of antiferromagnetic scattering of charge carriers at the interfaces between overlapping bound magnetic polarons from adjacent layers A and B.

Research Organization:
Univ. of Michigan, Ann Arbor, MI (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0008574; DMR-1237550; DMR-1561008; DMR-1428226; CHE-104008
OSTI ID:
1534441
Journal Information:
Chemistry of Materials, Vol. 28, Issue 23; ISSN 0897-4756
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 10 works
Citation information provided by
Web of Science

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Cited By (2)

Coherent magnetic nanoinclusions induce charge localization in half-Heusler alloys leading to high- T c ferromagnetism and enhanced thermoelectric performance journal January 2019
Phase Relations in the FeSe–FeGa2Se4–FeIn2Se4 System: Refinement of the Crystal Structures of FeIn2Se4 and FeGaInSe4 journal November 2019

Figures / Tables (12)

Figure 1(p. 2)figure Figure 1
Figure 2(p. 3)figure Figure 2
Figure 3(p. 4)figure Figure 3
Figure 4(p. 4)figure Figure 4
Table 1(p. 4)table Table 1
Figure 5(p. 5)figure Figure 5
Figure 6(p. 5)figure Figure 6
Figure 7(p. 5)figure Figure 7
Figure 8(p. 6)figure Figure 8
Figure 9(p. 7)figure Figure 9
Figure 10(p. 8)figure Figure 10
Figure 11(p. 8)figure Figure 11

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
36 MATERIALS SCIENCE
Chemistry
Materials science
Metals
Crystal structure
Layers
Magnetic properties
Electrical conductivity