Sensitivity of magnetic properties to chemical pressure in lanthanide garnets $Ln_3A_2X_3\text{O}_{12}$, $Ln$ = Gd, Tb, Dy, Ho, $A$ = Ga, Sc, In, Te, $X$ = Ga, Al, Li

TL;DR

This study investigates how chemical pressure influences the structural and magnetic properties of lanthanide garnets, revealing variations in magnetic ordering and magnetocaloric effects across different compositions and lanthanide ions.

Contribution

It provides a systematic analysis of magnetic behaviors and magnetocaloric properties in lanthanide garnets with various chemical compositions, highlighting the tuning of magnetic interactions and anisotropy.

Findings

Gd garnets show no magnetic ordering above 0.4 K.

Tb, Dy, Ho garnets exhibit magnetic ordering between 0.4 and 2.5 K.

Dy$_3$Ga$_5$O$_{12}$ shows superior magnetocaloric performance.

Abstract

A systematic study of the structural and magnetic properties of three-dimensionally frustrated lanthanide garnets $Ln_3A_2X_3\text{O}_{12}$, $Ln$ = Gd, Tb, Dy, Ho, $A$ = Ga, Sc, In, Te, $X$ = Ga, Al, Li is presented. Garnets with $Ln$ = Gd show magnetic behaviour consistent with isotropic Gd$^{3+}$ spins; no magnetic ordering is observed for T $\geq$ 0.4 K. Magnetic ordering features are seen for garnets with $Ln$ = Tb, Dy, Ho in the temperature range 0.4 < T < 2.5 K, however the nature of the magnetic ordering varies for the different $Ln$ as well as for different combinations of $A$ and $X$. The changes in magnetic behaviour can be explained by tuning of the magnetic interactions and changes in the single-ion anisotropy. The change in magnetic entropy is evaluated from isothermal magnetisation measurements to characterise the magnetocaloric effect in these materials. Among the Gd garnets, the maximum change in magnetic entropy per mole (15.45 J K$^{-1}$ mol$_{\text{Gd}}^{-1}$) is observed for Gd$_3$Sc$_2$Ga$_3$O$_{12}$ at 2 K, in a field of 9 T. The performance of Dy$_3$Ga$_5$O$_{12}$ as a magnetocaloric material surpasses the other garnets with $Ln$ = Tb, Dy, Ho.