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•Magnetic properties of both bulk and powder samples were studied.•Powder sample shows lower ΔSm but zero magnetic hysteresis compared to the bulk.•Strain plays a great role in the ...determination of ΔSm for first-order materials.•Peak value of ΔSm significantly enhances to 22 J kg−1K−1 at ΔH = 2 and T = 322 K.
The multi-component MnTX (T = Ni, Co; X = p-block elements) intermetallic system have attracted intensive attention due to their tunable magneto-structural phase transition and associated giant magnetocaloric effect. Here, we report an experimental study on the magnetic, magnetocaloric, and electrical properties of alloys that belong to the MnTX family- Mn0.5Fe0.5-xNi1+xSi0.94Al0.06. For all values of x (0≤ x ≤0.10), the materials exhibited a first-order magneto-structural phase transition from a low-temperature ferromagnetic orthorhombic phase to a high-temperature paramagnetic hexagonal phase. The transition was accompanied by large magnetic entropy changes of up to –22 and −57 J kg−1K−1 at T = 322 K for field changes of 2 T and 5 T, respectively. Most noticeably, a sharp jump in electrical resistivity was observed at T = 320 K for x = 0.1, which confirmed that the first-order phase transition preserved the mechanical stability of the material. The alloy with x = 0.1 was further crushed into powder and the magnetic properties were compared to its bulk counterpart. The enhanced mechanical stability and nearly zero magnetic hysteresis loss along with the fact that the system is constituted of cheap, non-toxic elements make this system worthy of consideration for near-room temperature magnetic refrigeration applications.
Materials responding vigorously to minor variations of external stimuli with negligible hysteresis could revolutionize many of the energy technologies, including refrigeration, actuation, and ...sensing. We report a combined experimental and theoretical study of a two-phase composite, naturally formed at the LaFe2Si stoichiometry, which exhibits a nearly anhysteretic, two-step first-order ferromagnetic-to-paramagnetic phase transformation with enhanced sensitivity to an external magnetic field. Other unusual properties include a large plateau-like positive magnetoresistance, magnetic-field-induced temperature and entropy changes occurring over a wide temperature range, and a Griffiths-like phase associated with short-range ferromagnetic clustering in the paramagnetic state. The heat capacity, magnetization, Mössbauer spectroscopy, and electrical resistivity, all exhibit characteristic, unusually sharp, first-order discontinuities even in magnetic fields as high as 100 kOe. We expect that similar phenomena could be designed in other mixed-phase systems, leading to novel functionalities, such as giant caloric effects in many yet undiscovered or/and underperforming intermetallic compounds.
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Combined experimental and density functional theory (DFT) study of Pr0.75Gd0.25ScGe and its hydride (Pr0.75Gd0.25ScGeH) reveals intricacies of composition-structure-property relationships in those ...distinctly layered compounds. Hydrogenation of the intermetallic parent, crystalizing in a tetragonal CeScSi-type structure, leads to an anisotropic volume expansion, that is, a(=b) lattice parameter decreases while the lattice expands along the c direction, yielding a net increase of cell volume. DFT calculations predict an antiparallel coupling of localized Gd and Pr magnetic moments in both materials at the ground state. While experiments corroborate this for the parent compound, there is no conclusive experimental proof for the hydride, where Pr moments do not order down to 3 K. DFT results also reveal that rare-earth – hydrogen interactions reduce spin-polarization of the Pr and Gd 5d and Sc 3d states at the Fermi energy, disrupt indirect exchange interactions mediated by conduction electrons, dramatically reduce the magnetic ordering temperature, and open a pseudo-gap in the majority-spin channel. Both experiments and theory show evidence of Kondo-like behavior in the hydride in the absence of an applied magnetic field, whereas increasing the field promotes magnetic ordering and suppresses Kondo-like behavior.
•Combined experimental and DFT investigation of structure-property relationships in Pr0.75Gd0.25ScGeH.•Hydrogen disrupts the magnetic exchange interactions allowing for competing Kondo interactions and magnetic fields.•DFT predicts antiparallel coupling of Pr and Gd at 0 K, however the Pr magnetic sublattice remains disordered down to 3 K.
Here this manuscript reports on the structural and magnetic properties of NdCuGa3 using powder and single crystal X-ray diffraction (XRD), zero-field single crystal neutron diffraction, ...magnetization, and specific heat measurements. Our XRD on a single crystal specimen of NdCuGa3 confirmed that it crystallizes in the tetragonal BaNiSi3-type structure. A magnetic phase transition at TN = 3.3 K is assessed using specific heat and ac magnetic susceptibility measurements. No additional anomaly below TN down to 50 mK was detected by performing specific heat measurements. Neutron single crystal diffraction data collected at T = 300 mK confirm the antiferromagnetic phase below TN= 3.3 K with the propagation vector $\vec{\tau}$ = (0.2, 0, 0). Possible magnetic structure solutions of NdCuGa3 are discussed
Future advancements in magnetocaloric refrigeration/heat pumping technologies depend on the discovery of new materials that demonstrate large, tunable magnetocaloric effects (MCEs) in the vicinity of ...coupled magnetic and structural phase transitions that occur reversibly with minimum hysteresis. Here, with this in mind, we investigate phase transitions, microstructure, magnetic, thermal, magnetocaloric, and transport properties of (Gd5-xScx)Si1.8Ge2.2 compounds. Replacement of magnetic Gd with non-magnetic Sc in Gd5-xScxSi1.8Ge2.2 increases the ferromagnetic to paramagnetic first order phase transition temperature, TC, with only a minor reduction in MCE when x ≤ 0.2. We also demonstrate that hydrostatic pressure further increases TC and reduces the hysteresis of the first order phase transition in Gd4.8Sc0.2Si1.8Ge2.2 from 7 to 4 K. Temperature-dependent x-ray powder diffraction study of Gd4.8Sc0.2Si1.8Ge2.2 confirms the monoclinic ↔ orthorhombic structural transformation at TC, in agreement with magnetic, calorimetric, and electrical transport measurements. In addition to the substantial magnetocaloric effect, a large magnetoresistance of ~20% is also observed in Gd4.8Sc0.2Si1.8Ge2.2 for ΔH = 50 kOe in the vicinity of the magnetostructural transition. Finally, in a drastic reversal of the initial doping behavior further additions of Sc (x > 0.2) suppress formation of the monoclinic phase, change the nature of the transition from first-to second-order, and reduce both the transition temperature and magnetocaloric effect.
Combined experimental and density functional theory (DFT) study of Pr0.75Gd0.25ScGe and its hydride (Pr0.75Gd0.25ScGeH) reveals intricacies of composition-structure-property relationships in those ...distinctly layered compounds. Hydrogenation of the intermetallic parent, crystalizing in a tetragonal CeScSi-type structure, leads to an anisotropic volume expansion, that is, a(=b) lattice parameter decreases while the lattice expands along the c direction, yielding a net increase of cell volume. DFT calculations predict an antiparallel coupling of localized Gd and Pr magnetic moments in both materials at the ground state. While experiments corroborate this for the parent compound, there is no conclusive experimental proof for the hydride, where Pr moments do not order down to 3 K. DFT results also reveal that rare-earth – hydrogen interactions reduce spin-polarization of the Pr and Gd 5d and Sc 3d states at the Fermi energy, disrupt indirect exchange interactions mediated by conduction electrons, dramatically reduce the magnetic ordering temperature, and open a pseudo-gap in the majority-spin channel. Here, both experiments and theory show evidence of Kondo-like behavior in the hydride in the absence of an applied magnetic field, whereas increasing the field promotes magnetic ordering and suppresses Kondo-like behavior.
We study crystal structure, phase transitions and magnetism of pseudo-binary TmxDy1-xAl2 (0 ≤ x ≤ 1) compounds using temperature dependent X-ray powder diffraction, specific heat and magnetization ...measurements, first principles, and model calculations. In low external magnetic fields, Dy-rich compounds undergo continuous, second-order phase transitions at the respective Curie temperatures, TC. In contrast, the Tm-rich compounds exhibit discontinuous, first-order anomalies in the magnetically ordered states. These sharp transitions correlate with a substantial energy difference between the room temperature cubic and ground state rhombohedral structures of TmAl2. A clear anomaly in the lattice parameter is observed at ∼30 K for x = 0.5, which nearly coincides with TC = 31.2 K. The effective quadrupolar moment of the lanthanides changes sign around x = 0.5, which leads to a nearly zero anisotropy constant and approximately spherical effective 4f charge densities, providing an explanation for the lack of structural distortions below TC for x = 0.5. The calculations confirm 001 as the easy magnetization axis in the ground state tetragonal structure of DyAl2, and reveal collapse of the orbital magnetic moment when the easy magnetization direction changes to 111. Within the rhombohedral ground state of TmAl2 111 is the easy magnetization direction.
•Investigated details phase transitions and magnetism of pseudo-binary TmxDy1-xAl2.•Observed complex evolution of both magnetic and lattice ground state structures with x.•Tm-rich compounds exhibit first-order anomalies in the magnetically ordered states.
Owing to the relative abundance of its constituent elements and large magnetocaloric properties observed near room temperature, the AlFe2B2 system has attracted much attention recently. Here, we have ...studied the magnetic and magnetocaloric properties of Al0.85+xSi0.15Fe2B2 (x = 0.2, 0.4) prepared by drop-casting followed by annealing and acid treatment. The second order ferromagnetic phase transitions were observed near room temperature (∼298–305 K) and peak magnetic entropy changes (−ΔSM) of more than −6 J kg−1 K−1 were observed for a field change of 5 T. The results are discussed in terms of the impurity phases formed in the compounds due to excess aluminum.
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