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تسجيل مستخدم جديدOrigin and tuning of the magnetocaloric effect for the magnetic refrigerant MnFe(P1-xGex)
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Neutron diffraction and magnetization measurements of the magneto refrigerant Mn1+yFe1-yP1-xGex reveal that the ferromagnetic and paramagnetic phases correspond to two very distinct crystal structures, with the magnetic entropy change as a function of magnetic field or temperature being directly controlled by the phase fraction of this first-order transition. By tuning the physical properties of this system we have achieved a maximum magnetic entropy change exceeding 74 J/Kg K for both increasing and decreasing field, more than twice the value of the previous record.
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The compounds, PrCo9Si4 and NdCo9Si4, have been recently reported to exhibit first-order ferromagnetic transitions near 24 K. We have subjected this compound for further characterization by magnetization, heat-capacity and electrical resistivity meas
urements at low temperatures in the presence of magnetic fields, particularly to probe magnetocaloric effect and magnetoresistance. The compounds are found to exhibit rather modest magnetocaloric effect at low temperatures peaking at Curie temperature, tracking the behavior of magnetoresistance. The magnetic transition does not appear to be first order in its character.
Magnetocaloric materials can be useful in magnetic refrigeration applications, but to be practical the magneto-refrigerant needs to have a very large magnetocaloric effect (MCE) near room temperature for modest applied fields (<2 Tesla) with small hy
steresis and magnetostriction, and should have a complete magnetic transition, be inexpensive, and environmentally friendly. One system that may fulfill these requirements is MnxFe2-xP1-yGey, where a combined first-order structural and magnetic transition occurs between the high temperature paramagnetic and low temperature ferromagnetic phase. We have used neutron diffraction, differential scanning calorimetry, and magnetization measurements to study the effects of Mn and Ge location in the structure on the ordered magnetic moment, MCE, and hysteresis for a series of compositions of the system near optimal doping. The diffraction results indicate that the Mn ions located on the 3f site enhance the desirable properties, while those located on the 3g sites are detrimental. The entropy changes measured directly by calorimetry can exceed 40 J/kg-K. The phase fraction that transforms, hysteresis of the transition, and entropy change can be controlled by both the compositional homogeneity and the particle size, and an annealing procedure has been developed that substantially improves the performance of all three properties of the material. On the basis of these results we have identified a pathway to optimize the MCE properties of this system for magnetic refrigeration applications.
An approach to adjusting the conduction band population for tuning the magnetic and magnetocaloric response of EuO1-{delta} thin films through control of oxygen vacancies ({delta} = 0, 0.025, and 0.09) is presented. The films each showed a paramagnet
ic to ferromagnetic transition around 65 K, with an additional magnetic ordering transition at higher temperatures in the oxygen deficient samples. All transitions are observed to be of second order. A maximum magnetic entropy change of 6.4 J/kg K over a field change of 2 T with a refrigerant capacity of 223 J/kg was found in the sample with {delta} = 0, and in all cases the refrigerant capacities of the thin films under study were found to exceed that reported for bulk EuO. Adjusting the oxygen content was shown to produce table-like magnetocaloric effects, desirable for ideal Ericsson-cycle magnetic refrigeration. These films are thus excellent candidates for small-scale magnetic cooling technology in the liquid nitrogen temperature range.
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 $T_C$.
Neutron powder diffraction studies of the crystal and magnetic structures of the magnetocaloric compound Mn1.1Fe0.9(P0.8Ge0.2) have been carried out as a function of temperature, applied magnetic field, and pressure. The data reveal that there is onl
y one transition observed over the entire range of variables explored, which is a combined magnetic and structural transformation between the paramagnetic to ferromagnetic phases (Tc~255 K for this composition). The structural part of the transition is associated with an expansion of the hexagonal unit cell in the direction of the a- and b-axes and a contraction of the c-axis as the FM phase is formed, which originates from an increase in the intra-layer metal-metal bond distance. The application of pressure is found to have an adverse effect on the formation of the FM phase since pressure opposes the expansion of the lattice and hence decreases Tc. The application of a magnetic field, on the other hand, has the expected effect of enhancing the FM phase and increasing Tc. We find that the substantial range of temperature/field/pressure coexistence of the PM and FM phases observed is due to compositional variations in the sample. In-situ high temperature diffraction measurements were carried out to explore this issue, and reveal a coexisting liquid phase at high temperatures that is the origin of this variation. We show that this range of coexisting phases can be substantially reduced by appropriate heat treatment to improve the sample homogeneity.
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