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Register a new userHeterogeneous nucleation and heat flux avalanches in La(Fe,Si)$_{13}$ magnetocaloric compounds near the critical point
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The phase transformation kinetics of LaFe$_{11.41}$Mn$_{0.30}$Si$_{1.29}$-H$_{1.65}$ magnetocaloric compound is addressed by low rate calorimetry experiments. Scans at 1 mK/s show that its first order phase transitions are made by multiple heat fllux avalanches. Getting very close to the critical point, the step-like discontinuous behavior associated with avalanches is smoothed out and thermal hysteresis disappears. This result is confirmed by magneto-resistivity measurements and allows to measure accurate values of the zero field hysteresis ($Delta T_{hyst}$ = 0.37 K) and of the critical field (H$_c$ = 1.19 T). The number and magnitude of heat flux avalanches change with magnetic field, showing the interplay between the intrinsic energy barrier between phases and the microstructural disorder of the sample.
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We study heat flux avalanches occurring at the first order transition in La(Fe-Mn-Si)$_{13}$-H$_{1.65}$ magnetocaloric material. As the transition is associated to the phase boundaries motion that gives rise to the latent heat, we develop a non equilibrium thermodynamic model. By comparing the model with experimental calorimetry data available for Mn=0.18, we find the values of the intrinsic kinetic parameter $R_L$, expressing the damping for the moving boundary interface, at different magnetic fields. We conclude that by increasing field, thus approaching the critical point, the avalanches increase in number and their kinetics is slowed down.
We compute the magnetocaloric effect (MCE) in the GdTX (T=Sc, Ti, Co, Fe; X=Si, Ge) compounds as a function of the temperature and the external magnetic field. To this end we use a density functional theory approach to calculate the exchange-coupling interactions between Gd$^{3+}$ ions on each compound. We consider a simplified magnetic Hamiltonian and analyze the dependence of the exchange couplings on the transition metal T, the p-block element X, and the crystal structure (CeFeSi-type or CeScSi-type). The most significant effects are observed for the replacements Ti $to$ Sc or Fe $to$ Co which have an associated change in the parity of the electron number in the 3d level. These replacements lead to an antiferromagnetic contribution to the magnetic couplings that reduces the Curie temperature and can even lead to an antiferromagnetic ground state. We solve the magnetic models through mean field and Monte Carlo calculations and find large variations among compounds in the magnetic transition temperature and in the magnetocaloric effect, in agreement with the available experimental data. The magnetocaloric effect shows a universal behavior as a function of temperature and magnetic field in the ferromagnetic compounds after a scaling of the relevant energy scales by the Curie temperature $T_C$.
Magnetocaloric effect and magnetoresistance have been studied in Dy(Co1-xSix)2 [x=0, 0.075 and 0.15] compounds. Magnetocaloric effect has been calculated in terms of adiabatic temperatue change (Delta Tad) as well as isothermal magnetic entropy change (Delta SM) using the heat capacity data. The maximum values of DeltaSM and DeltaTad for DyCo2 are found to be 11.4 JKg-1K-1 and 5.4 K, respectively. Both DSM and DTad decrease with Si concentration, reaching a value of 5.4 JKg-1K-1 and 3 K, respectively for x=0.15. The maximum magnetoresistance is found to about 32% in DyCo2, which decreases with increase in Si. These variations are explained on the basis of itinerant electron metamagnetism occurring in these compounds.
Large thermal hysteresis in the MnFe(P, Si, B) system hinders the heat exchange rate and thus limits the magnetocaloric applications at high frequencies. Substitution of Mn by V in Mn1-xVxFe0.95P0.593Si0.33B0.077 and Mn1-xVxFe0.95P0.563Si0.36B0.077 alloys was found to reduce the thermal hysteresis due to a decrease in the latent heat. Introducing V increases both the field-induced transition temperature shift and the magnetic moment per formula unit. Thus, a decease in the thermal hysteresis is obtained without losing the giant magnetocaloric effect. In consequence, an ultralow hysteresis (0.7 K) and a giant adiabatic temperature change of 2.3 K were achieved, which makes these alloys promising candidates for commercial magnetic refrigerator using permanent magnets.
We present a study of the magnetoresistance, the specific heat and the magnetocaloric effect of equiatomic $RET$Mg intermetallics with $RE = {rm La}$, Eu, Gd, Yb and $T = {rm Ag}$, Au and of GdAuIn. Depending on the composition these compounds are paramagnetic ($RE = {rm La}$, Yb) or they order either ferro- or antiferromagnetically with transition temperatures ranging from about 13 to 81 K. All of them are metallic, but the resistivity varies over 3 orders of magnitude. The magnetic order causes a strong decrease of the resistivity and around the ordering temperature we find pronounced magnetoresistance effects. The magnetic ordering also leads to well-defined anomalies in the specific heat. An analysis of the entropy change leads to the conclusions that generally the magnetic transition can be described by an ordering of localized $S=7/2$ moments arising from the half-filled $4f^7$ shells of Eu$^{2+}$ or Gd$^{3+}$. However, for GdAgMg we find clear evidence for two phase transitions indicating that the magnetic ordering sets in partially below about 125 K and is completed via an almost first-order transition at 39 K. The magnetocaloric effect is weak for the antiferromagnets and rather pronounced for the ferromagnets for low magnetic fields around the zero-field Curie temperature.
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