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

Journal Article · · Journal of Alloys and Compounds
 [1];  [1];  [2];  [3];  [4];  [5]
  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)

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.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC); Ministry of Science and Technology of the People's Republic of China
Grant/Contract Number:
AC02-06CH11357
OSTI ID:
1618451
Alternate ID(s):
OSTI ID: 1701869
Journal Information:
Journal of Alloys and Compounds, Journal Name: Journal of Alloys and Compounds Journal Issue: C Vol. 808; ISSN 0925-8388
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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