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Register a new userEnhanced magnetocaloric effect from Cr substitution in Ising lanthanide gallium garnets $Ln_3text{CrGa}_4text{O}_{12}$ ($Ln$ = Tb, Dy, Ho)
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A detailed study on the crystal structure and bulk magnetic properties of Cr substituted Ising type lanthanide gallium garnets $Ln_3text{CrGa}_4text{O}_{12}$ ($Ln$ = Tb, Dy, Ho) has been carried out using room temperature powder X-Ray and neutron diffraction, magnetic susceptibility, isothermal magnetisation and heat capacity measurements. The magnetocaloric effect (MCE) in $Ln_3text{CrGa}_4text{O}_{12}$ is compared to that of $Ln_3text{Ga}_5text{O}_{12}$. In lower magnetic fields attainable by a permanent magnet ($leq$ 2 T), Cr substitution greatly enhances the MCE by 20% for $Ln$ = Dy and 120% for $Ln$ = Ho compared to the unsubstituted $Ln_3text{Ga}_5text{O}_{12}$. This is likely due to changes in the magnetic ground state as Cr substitution also significantly reduces the frustration in the magnetic lattice for the Ising type $Ln_3text{Ga}_5text{O}_{12}$.
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The lanthanide orthoborates, $Ln$BO$_3$, $Ln$ = Gd, Tb, Dy, Ho, Er, Yb crystallise in a monoclinic structure with the magnetic $Ln^{3+}$ forming an edge-sharing triangular lattice. The triangles are scalene, however all deviations from the ideal equilateral geometry are less than 1.5%. The bulk magnetic properties are studied using magnetic susceptibility, specific heat and isothermal magnetisation measurements. Heat capacity measurements show ordering features at $T leq$ 2 K for $Ln$ = Gd, Tb, Dy, Er. No ordering is observed for YbBO$_3$ at $T geq$ 0.4 K and HoBO$_3$ is proposed to have a non-magnetic singlet state. Isothermal magnetisation measurements indicate isotropic Gd$^{3+}$ spins and strong single-ion anisotropy for the other $Ln^{3+}$. The change in magnetic entropy has been evaluated to determine the magnetocaloric effect in these materials. GdBO$_3$ and DyBO$_3$ are found to be competitive magnetocaloric materials in the liquid helium temperature regime.
A systematic study of the structural and magnetic properties of three-dimensionally frustrated lanthanide garnets $Ln_3A_2X_3text{O}_{12}$, $Ln$ = 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.
The interplay of charge, spin, orbital and lattice degrees of freedom has recently received great interest due to its potential to improve the magnetocaloric effect (MCE) for the purpose of magnetic cooling applications. Here we propose a new mechanism for a giant inverse MCE in rare-earth tetraborides, especially for Ho1-xDyxB4 (x = 0.0, 0.5, and 1.0). For x = 0.0, 0.5, and 1.0, the maximum entropy changes of the giant inverse MCE are found to be 22.7 J/kgK, 19.6 J/kgK, and 19.0 J/kgK with critical fields of 25 kOe, 40 kOe, and 50 kOe, respectively. It is remarkable that such a giant MCE is realized, even when applying a low magnetic field, which enables a field-tuned entropy change and brings about a significant advantage for several applications. For all compounds, we have systematically studied how the entropy changes as a function of the field and temperature and investigated their correlation with consecutive double transitions, i.e., the magnetic dipolar order at T = TN and the quadrupolar order at T = TQ (TQ < TN). We found that the maximum entropy change occurs at T = TQ and the critical field associated with the meta-magnetic transition, which is in good agreement with the experimental data. Thus, we elucidate that this unique behaviour is attributed to the strong coupling between magnetic dipoles and quadrupoles in the presence of strong spin-orbit coupling and geometric frustration. Our work offers new insights into both the academic interest of multipolar degrees of freedom in magnetic materials and the discovery of giant MCE with various applications for magnetic cooling systems.
The magnetic and thermodynamic properties of the complete Ln$_{2/3}$Cu$_3$Ti$_4$O$_{12}$ series were investigated. Here $Ln$ stands for the lanthanides La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, and Yb. %Most of the compounds were prepared as single phase polycrystalline powder %without any traces of impurities. Marginal amounts of %impurities $(< 2%)$ were detected $Ln=$ Gd, Er, and Tm. %Significant amounts of impurity phases were found for $Ln=$ Ce and Yb. All the samples investigated crystallize in the space group $Imbar{3}$ with lattice constants that follow the lanthanide contraction. The lattice constant of the Ce compound reveals the presence of Ce$^{4+}$ leading to the composition Ce$_{1/2}$Cu$_3$Ti$_4$O$_{12}$. From magnetic susceptibility and electron-spin resonance experiments it can be concluded that the copper ions always carry a spin $S=1/2$ and order antiferromagnetically close to 25,K. The Curie-Weiss temperatures can approximately be calculated assuming a two-sublattice model corresponding to the copper and lanthanide ions, respectively. It seems that the magnetic moments of the heavy rare earths are weakly coupled to the copper spins, while for the light lanthanides no such coupling was found. The $4f$ moments remain paramagnetic down to the lowest temperatures, with the exception of the Tm compound, which indicates enhanced Van-Vleck magnetism due to a non-magnetic singlet ground state of the crystal-field split $4f$ manifold. From specific-heat measurements we accurately determined the antiferromagnetic ordering temperature and obtained information on the crystal-field states of the rare-earth ions. The heat-capacity results also revealed the presence of a small fraction of Ce$^{3+}$ in a magnetic $4f^1$ state.
Recently, a massive magnetocaloric effect near the liquefaction temperature of hydrogen has been reported in the ferromagnetic material HoB$_{2}$. Here we investigate the effects of Dy substitution in the magnetocaloric properties of Ho$_{1-x}$Dy$_{x}$B$_{2}$ alloys ($textit{x}$ = 0, 0.3, 0.5, 0.7, 1.0). We find that the Curie temperature ($textit{T}$$_{C}$) gradually increases upon Dy substitution, while the magnitude of the magnetic entropy change |$Delta textit{S}_{M}$| at $textit{T}$ = $textit{T}_{C}$ decreases from 0.35 to 0.15 J cm$^{-3}$ K$^{-1}$ for a field change of 5 T. Due to the presence of two magnetic transitions in these alloys, despite the change in the peak magnitude of |$Delta textit{S}_{M}$|, the refrigerant capacity ($textit{RC}$) and refrigerant cooling power ($textit{RCP}$) remains almost constant in all doping range, which as large as 5.5 J cm$^{-3}$ and 7.0 J cm$^{-3}$ for a field change of 5 T. These results imply that this series of alloys could be an exciting candidate for magnetic refrigeration in the temperature range between 10-50 K.
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