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Title: Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5

Abstract

Crystal structure and magnetic properties of Gd5Si1.5Ge2.5 and Gd4.9Zr0·1Si1.5Ge2.5 were investigated using high-energy X-ray diffraction and magnetic measurements. Results showed that a Zr substitution for 2% Gd reduces unit cell volumes of a room-temperature monoclinic and a low-temperature orthorhombic lattice and a difference between them at a magnetostructural transition. At a microscopic level, the Zr substitution increases length of disconnected interlayer T–T bonds of the monoclinic lattice at the expense of length of connected interlayer T–T bonds (T = Si, Ge). These opposing changes of the interlayer T–T bonds provided evidence for existence of a short-range chemical order of Ge atoms in lattices of Gd5Si1.5Ge2.5 and its weakening by the Zr substitution. Magnetic measurements revealed that the Zr substitution brings about a change of the magnetic structure and a reduction of a giant magnetocaloric effect of Gd5Si1.5Ge2.5. Based on such structural and magnetic changes due to the Zr substitution, we propose a relation between the short-range chemical order and the total entropy change at the magnetostructural transition. Finally, using this relation, a giant magnetocaloric effect and an annealing effect observed over a wide range of Gd5(Si,Ge)4 composition can be explained quantitatively.

Authors:
 [1]; ORCiD logo [1]; ORCiD logo [2];  [3];  [4];  [5]
+ Show Author Affiliations
  1. Northeastern Univ., Shenyang (China)
  2. Beijing Inst. of Technology (China)
  3. Univ. of Science and Technology, Beijing (China)
  4. Northern Illinois Univ., De Kalb, IL (United States)
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC); Ministry of Science and Technology of the People's Republic of China
OSTI Identifier:
1618451
Alternate Identifier(s):
OSTI ID: 1701869
Grant/Contract Number:  
AC02-06CH11357; 51831003; 2012CB619405; DE–AC02–06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Alloys and Compounds
Additional Journal Information:
Journal Volume: 808; Journal Issue: C; Journal ID: ISSN 0925-8388
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Synchrotron radiation; crystal structure; magnetocaloric effect; rare earth compound; x-ray diffraction

Citation Formats

Kou, Ronghui, Gao, Jianrong, Nie, Zhihua, Wang, Yandong, Brown, Dennis E., and Ren, Yang. Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5. United States: N. p., 2019. Web. doi:10.1016/j.jallcom.2019.151751.
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Kou, Ronghui, Gao, Jianrong, Nie, Zhihua, Wang, Yandong, Brown, Dennis E., & Ren, Yang. Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5. United States. https://doi.org/10.1016/j.jallcom.2019.151751
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Kou, Ronghui, Gao, Jianrong, Nie, Zhihua, Wang, Yandong, Brown, Dennis E., and Ren, Yang. Wed . "Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5". United States. https://doi.org/10.1016/j.jallcom.2019.151751. https://www.osti.gov/servlets/purl/1618451.
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@article{osti_1618451,
title = {Evidence for a short-range chemical order of Ge atoms and its critical role in inducing a giant magnetocaloric effect in Gd5Si1.5Ge2.5},
author = {Kou, Ronghui and Gao, Jianrong and Nie, Zhihua and Wang, Yandong and Brown, Dennis E. and Ren, Yang},
abstractNote = {Crystal structure and magnetic properties of Gd5Si1.5Ge2.5 and Gd4.9Zr0·1Si1.5Ge2.5 were investigated using high-energy X-ray diffraction and magnetic measurements. Results showed that a Zr substitution for 2% Gd reduces unit cell volumes of a room-temperature monoclinic and a low-temperature orthorhombic lattice and a difference between them at a magnetostructural transition. At a microscopic level, the Zr substitution increases length of disconnected interlayer T–T bonds of the monoclinic lattice at the expense of length of connected interlayer T–T bonds (T = Si, Ge). These opposing changes of the interlayer T–T bonds provided evidence for existence of a short-range chemical order of Ge atoms in lattices of Gd5Si1.5Ge2.5 and its weakening by the Zr substitution. Magnetic measurements revealed that the Zr substitution brings about a change of the magnetic structure and a reduction of a giant magnetocaloric effect of Gd5Si1.5Ge2.5. Based on such structural and magnetic changes due to the Zr substitution, we propose a relation between the short-range chemical order and the total entropy change at the magnetostructural transition. Finally, using this relation, a giant magnetocaloric effect and an annealing effect observed over a wide range of Gd5(Si,Ge)4 composition can be explained quantitatively.},
doi = {10.1016/j.jallcom.2019.151751},
journal = {Journal of Alloys and Compounds},
number = C,
volume = 808,
place = {United States},
year = {2019},
month = {8}
}
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https://doi.org/10.1016/j.jallcom.2019.151751
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Cited by: 6 works
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Figures / Tables:

Table 1 Table 1: Comparison of previously measured and predicted total entropy changes of Gd5(Si,Ge)4 composition at a magnetic field change from 0 to 5 T. Measured data are taken from Refs. [9,14].
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