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Intense ferromagnetic fluctuations preceding magnetoelastic first-order transitions in giant magnetocaloric LaFe13−xSix

Zhao Zhang1,2, Houbo Zhou3,4, Richard Mole5, Chenyang Yu1,2, Zhe Zhang1,2, Xinguo Zhao1, Weijun Ren1, Dehong Yu5,*, Bing Li1,2,† et al.

Fengxia Hu3,4,‡, Baogen Shen3,4, and Zhidong Zhang1,2

  • 1Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, 72 Wenhua Road, Shenyang, Liaoning 110016, China
  • 2School of Materials Science and Engineering, University of Science and Technology of China, 72 Wenhua Road, Shenyang, Liaoning 110016, China
  • 3Beijing National Laboratory for Condensed Matter Physics and State Key Laboratory of Magnetism, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China
  • 4School of Physical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China
  • 5Australian Nuclear Science and Technology Organisation, Locked Bag 2001, Kirrawee DC NSW 2232, Australia

  • *dyu@ansto.gov.au
  • †bingli@imr.ac.cn
  • ‡fxhu@iphy.ac.cn

Phys. Rev. Materials 5, L071401 – Published 22 July, 2021

DOI: https://doi.org/10.1103/PhysRevMaterials.5.L071401

Abstract

First-order magnetic transitions are of both fundamental and technological interest given that a number of emergent phases and functionalities are thereby created. Of particular interest are giant magnetocaloric effects, which are attributed to first-order magnetic transitions and have attracted broad attention for solid-state refrigeration applications. While the conventional wisdom is that atomic lattices play an important role in first-order magnetic transitions, a coherent microscopic description of the lattice and spin degrees of freedom is still lacking. Here, we present a comparative neutron scattering study on the lattice and spin dynamics in intermetallic LaFe11.6Si1.4 and LaFe11.2Si1.8, which represent one of the most classical giant magnetocaloric systems and undergo first-order and second-order magnetic transitions, respectively. While their spin-phonon coupling effects are quite similar, LaFe11.6Si1.4 exhibits a much stronger magnetic diffuse scattering in the paramagnetic state preceding its first-order magnetic transition, corresponding to intense ferromagnetic fluctuations. These dynamic insights suggest that the magnetic degree of freedom dominates this magnetoelastic transition and ferromagnetic fluctuations might be universally relevant for this kind of compounds.

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