Tuning the giant inverse magnetocaloric effect in Mn2?xCrxSb compounds

Structural, magnetic, and magnetocaloric properties of Mn2-xCrxSb compounds have been studied. In these compounds, a first order magnetic phase transition from the ferrimagnetic to the antiferromagnetic state occurs with decreasing temperature, giving rise to giant inverse magnetocaloric effects that can be tuned over a wide temperature interval through changes in substitution concentration. Entropy changes as high as 7.5?J/kg?K have been observed, and a composition independent entropy change is obtained for several different concentrations/working temperatures, making these compounds suitable candidates for a composite working material.RST/Radiation, Science and TechnologyApplied Science

Thermal-history dependent magnetoelastic transition in (Mn,Fe)2(P,Si)

The thermal-history dependence of the magnetoelastic transition in (Mn,Fe)2(P,Si) compounds has been investigated using high-resolution neutron diffraction. As-prepared samples display a large difference in paramagnetic-ferromagnetic (PM-FM) transition temperature compared to cycled samples. The initial metastable state transforms into a lower-energy stable state when the as-prepared sample crosses the PM-FM transition for the first time. This additional transformation is irreversible around the transition temperature and increases the energy barrier which needs to be overcome through the PM-FM transition. Consequently, the transition temperature on first cooling is found to be lower than on subsequent cycles characterizing the so-called “virgin effect.” High-temperature annealing can restore the cycled sample to the high-temperature metastable state, which leads to the recovery of the virgin effect. A model is proposed to interpret the formation and recovery of the virgin effect.RST/Radiation, Science and TechnologyApplied Science

Effect of Carbon Doping on the Structure and Magnetic Phase Transition in (Mn,Fe₂(P,Si))

Given the potential applications of (Mn,Fe2(P,Si))-based materials for room-temperature magnetic refrigeration, several research groups have carried out fundamental studies aimed at understanding the role of the magneto-elastic coupling in the first-order magnetic transition and further optimizing this system. Inspired by the beneficial effect of the addition of boron on the magnetocaloric effect of (Mn,Fe2(P,Si))-based materials, we have investigated the effect of carbon (C) addition on the structural properties and the magnetic phase transition of Mn 1.25Fe 0.70P 0.50Si 0.50C z and Mn 1.25Fe 0.70P 0.55Si 0.45C z compounds by x-ray diffraction, neutron diffraction and magnetic measurements in order to find an additional control parameter to further optimize the performance of these materials. All samples crystallize in the hexagonal Fe 2P -type structure (space group P-62m), suggesting that C doping does not affect the phase formation. It is found that the Curie temperature increases, while the thermal hysteresis and the isothermal magnetic entropy change decrease by adding carbon. Room-temperature neutron diffraction experiments on Mn 1.25Fe 0.70P 0.55Si 0.45C z compounds reveal that the added C substitutes P/Si on the 2c site and/or occupies the 6k interstitial site of the hexagonal Fe 2P -type structure.RST/Fundamental Aspects of Materials and EnergyRST/Neutron and Positron Methods in Material

Tuning the phase transition in transition-metal-based magnetocaloric compounds

Neutron-diffraction experiments on the (Mn,Fe)2(P,Si)-type compounds have shown a site preference of Si atoms in the hexagonal structure. The degree of ordering of Si depends on the Si/P ratio, while it is independent of the Mn/Fe ratio. The ferromagnetic-paramagnetic magnetoelastic transition is closely related to the size of the magnetic moment on the 3f site. A preferred occupation of Si atoms on the 2c site stabilizes and decreases the magnetic moment on the 3f and 3g site, respectively, which is supported by our first-principles density functional theory calculations. This effect, together with the contribution from the Si substitution-induced changes in the interatomic distances, leads to a phase transition that is tunable in temperature and degree of first order in Mn1.25Fe0.70P1?xSix compounds. These results provide us with further insight into the relationship between the magnetoelastic phase transition and the local atomic coordination.RST/Radiation, Science and TechnologyApplied Science

Spin correlations in (Mn,Fe)2(P,Si) magnetocaloric compounds above Curie temperature

The longitudinal-field muon-spin relaxation (LF-μSR) technique was employed to study the spin correlations in (Mn,Fe)2(P,Si) compounds above the ferromagnetic transition temperature (TC). The (Mn,Fe)2(P,Si) compound under study is found to show itinerant magnetism. The standard deviation of the magnetic field distribution of electronic origin increases with a decrease in temperature, which is attributed to the development of spin correlations. The anomalously low magnetic fluctuation rate is suggested to be another signature of the spin correlations. The development of pronounced magnetic fluctuations is in agreement with the observed deviation of the paramagnetic susceptibility from Curie–Weiss behavior. Our study sheds light on the magneto-elastic transition and the mixed magnetism in (Mn,Fe)2(P,Si) compounds.RST/Fundamental Aspects of Materials and Energ

Efficient Room-Temperature Cooling with Magnets

Magnetic cooling is a highly efficient refrigeration technique with the potential to replace the traditional vapor compression cycle. It is based on the magnetocaloric effect, which is associated with the temperature change of a material when placed in a magnetic field. We present experimental evidence for the origin of the giant entropy change found in the most promising materials, in the form of an electronic reconstruction caused by the competition between magnetism and bonding. The effect manifests itself as a redistribution of the electron density, which was measured by X-ray absorption and diffraction on MnFe(P,Si,B). The electronic redistribution is consistent with the formation of a covalent bond, resulting in a large drop in the Fe magnetic moments. The simultaneous change in bond length and strength, magnetism, and electron density provides the basis of the giant magnetocaloric effect. This new understanding of the mechanism of first order magneto-elastic phase transitions provides an essential step for new and improved magnetic refrigerants.RST/Fundamental Aspects of Materials and Energ

Combined effect of annealing temperature and vanadium substitution for mangetocaloric Mn_1.2-xV_xFe_0.75P_0.5Si_0.5 alloys

Approaching the border of the first order transition and second order transition is significant to optimize the giant magnetocaloric materials performance. The influence of vanadium substitution in the Mn1.2-xVxFe0.75P0.5Si0.5 alloys is investigated for annealing temperatures of 1323, 1373 and 1423 K. By tuning both the annealing temperature and the V substitution simultaneously, the magnetocaloric effect can be enhanced without enlarging the thermal hysteresis near the border of the first to second order transition. Neutron diffraction measurements reveal the changes of site occupation and interatomic distances caused by varying the annealing temperature and V substitution. The properties of the alloy with x = 0.02 annealed at 1323 K is comparable to those found for the MnFe0.95P0.595Si0.33B0.075 alloy, illustrating that Mn1.2-xVxFe0.75P0.5Si0.5 alloys are excellent materials for magnetic heat-pumping near room temperature.RST/Fundamental Aspects of Materials and EnergyQRD/Kouwenhoven LabRST/Neutron and Positron Methods in Material

Kinetic-arrest-induced phase coexistence and metastability in (Mn,Fe)2(P,Si)

Neutron diffraction, Mössbauer spectroscopy, magnetometry, and in-field x-ray diffraction are employed to investigate the magnetoelastic phase transition in hexagonal (Mn,Fe)2(P,Si) compounds. (Mn,Fe)2(P,Si) compounds undergo for certain compositions a second-order paramagnetic (PM) to a spin-density-wave (SDW) phase transition before further transforming into a ferromagnetic (FM) phase via a first-order phase transition. The SDW-FM transition can be kinetically arrested, causing the coexistence of FM and untransformed SDW phases at low temperatures. Our in-field x-ray diffraction and magnetic relaxation measurements clearly reveal the metastability of the untransformed SDW phase. This unusual magnetic configuration originates from the strong magnetoelastic coupling and the mixed magnetism in hexagonal (Mn,Fe)2(P,Si) compounds.RST/Fundamental Aspects of Materials and EnergyTechnici Poo

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Short-range magnetic correlations and spin dynamics in the paramagnetic regime of (Mn,Fe)2(P,Si)

The spatial and temporal correlations of magnetic moments in the paramagnetic regime of (Mn,Fe)2(P,Si) have been investigated by means of polarized neutron diffraction and muon-spin relaxation techniques. Short-range magnetic correlations are present at temperatures far above the ferromagnetic transition temperature (TC). This leads to deviations of paramagnetic susceptibility from Curie-Weiss behavior. These short-range magnetic correlations extend in space, slow down with decreasing temperature, and finally develop into long-range magnetic order at TC.RST/Fundamental Aspects of Materials and EnergyRST/Neutron and Positron Methods in Material