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Comparative study of magnetocaloric properties for Gd3+ compounds with different frustrated lattice geometries

Authors: Koskelo, Eliseanne; Mukherjee, Paromita; Liu, Cheng; Sackville Hamilton, Alice; Ong, Harapan; Castelnovo, Claudio; Zhitomirsky, M.E.; +1 Authors

Comparative study of magnetocaloric properties for Gd3+ compounds with different frustrated lattice geometries

Abstract

As materials with suppressed ordering temperatures and enhanced ground state entropies, frustrated magnetic oxides are ideal candidates for cryogenic magnetocaloric refrigeration. While previous materials design has focused on tuning the magnetic moments, their interactions, and density of moments on the lattice, there has been relatively little attention to frustrated lattices. Prior theoretical work has shown that the magnetocaloric cooling rate at the saturation field is proportional to a macroscopic number of soft mode excitations that arise due to the classical ground state degeneracy. The number of these modes is directly determined by the geometry of the frustrating lattice. For corner-sharing geometries, the pyrochlore has 50\% more modes than the garnet and kagome lattices, whereas the edge-sharing \emph{fcc} has only a subextensive number of soft modes. Here, we study the role of soft modes in the magnetocaloric effect of four large-spin Gd$^{3+}$ ($L=0$, $J=S=7/2$) Heisenberg antiferromagnets on a kagome, garnet, pyrochlore, and \emph{fcc} lattice. By comparing measurements of the magnetic entropy change $ΔS_m$ of these materials at fields up to $9$~T with predictions using mean-field theory and Monte Carlo simulations, we are able to understand the relative importance of spin correlations and quantization effects. We observe that tuning the value of the nearest neighbor coupling has a more dominant contribution to the magnetocaloric entropy change in the liquid-He cooling regime ($2$-$20$~K), rather than tuning the number of soft mode excitations. Our results inform future materials design in terms of dimensionality, degree of magnetic frustration, and lattice geometry.

15 pages, 14 figures

Countries
United Kingdom, France
Keywords

[PHYS]Physics [physics], TK1001-1841, Condensed Matter - Materials Science, 4902 Mathematical Physics, Strongly Correlated Electrons (cond-mat.str-el), 34 Chemical Sciences, [SPI] Engineering Sciences [physics], TJ807-830, Materials Science (cond-mat.mtrl-sci), FOS: Physical sciences, Renewable energy sources, [PHYS] Physics [physics], [SPI]Engineering Sciences [physics], Condensed Matter - Strongly Correlated Electrons, Production of electric energy or power. Powerplants. Central stations, 49 Mathematical Sciences

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citations
This is an alternative to the "Influence" indicator, which also reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Citations provided by BIP!
popularity
This indicator reflects the "current" impact/attention (the "hype") of an article in the research community at large, based on the underlying citation network.
BIP!Popularity provided by BIP!
influence
This indicator reflects the overall/total impact of an article in the research community at large, based on the underlying citation network (diachronically).
BIP!Influence provided by BIP!
impulse
This indicator reflects the initial momentum of an article directly after its publication, based on the underlying citation network.
BIP!Impulse provided by BIP!
0
Average
Average
Average
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gold