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  1. Balancing performance of active magnetic regenerators: a comprehensive experimental study of aspect ratio, particle size, and operating conditions

    Abstract Effective and, at the same time, efficient active magnetic regenerator (AMR) performance requires balanced geometry and operating conditions. Here the influence of regenerator shape, magnetocaloric material size, operating frequency, and utilization on the performance of gadolinium packed-particle bed AMRs is demonstrated experimentally. Various metrics are applied to assess effectiveness and efficiency. Observed temperature spans and cooling powers across a wide range of operating conditions are used to evaluate system performance and estimate exergetic cooling power and exergetic power quotient. A new metric combining exergetic cooling power and pump power provides an estimate of the maximum achievable second law efficiency.more » Five regenerator geometries with equal volumes and the aspect ratio from 1.0 to 3.8, and four different ranges of Gd spherical particles between 182 and 354 µ m, are investigated. Improvements in system performance are demonstrated by a boost in specific cooling power of gadolinium from 0.85 to 1.16 W g −1 and maximum temperature span from 8.9 to 15.1 K. The optimum exergetic cooling power is observed for 1.37 utilization and 3 Hz operating frequency, exergetic power quotient exhibits a maximum at the same utilization but at 2 Hz frequency, while the highest efficiency is recorded at 1 Hz and utilization of 0.5, demonstrating that multiple performance metrics must be balanced to achieve regenerator design meeting all performance targets.« less
  2. Ground-state degeneracy and complex magnetism of geometrically frustrated Gd 2 Ir 0.97 Si 2.97

    We report a new triangular-lattice intermetallic compound Gd2Ir0.97Si2.97 was successfully synthesized as single phase by deliberately introducing vacancies. Theoretical analysis suggests that the ground state is competing with several low-energy spin configurations due to magnetic frustration on a nearly ideal triangular lattice. Despite a number of competing magnetic states, the compound exhibits long-range antiferromagnetic order at16K, a long-range ferrimagnetic transition at 6.5 K, and a reentrant cluster-glass transition below Tf ~ 3K. The complex magnetism in the compound could be correlated with competing antiferromagnetic and ferrimagnetic structures predicted theoretically.
  3. Unusual first-order magnetic phase transition and large magnetocaloric effect in Nd2In

    A large magnetocaloric effect with its maximum near the boiling point of natural gas occurs in a rare-earth intermetallic compound Nd2In. While behaviors of physical properties indicate that paramagnetic-ferromagnetic transformation supporting the large magnetocaloric effect is firstorder in nature, temperature dependent crystallographic study reveals no changes in lattice symmetry and lack of discontinuities either in phase volume or lattice parameters. In this work we discuss how the borderline first-order nature of phase transformation in Nd2In is markedly different from conventional firstorder magnetic transitions occurring in other members of the family – isostructural Pr2In and non-isostructural Eu2In.
  4. Fathoming the anisotropic magnetoelasticity and magnetocaloric effect in GdNi

    Intermetallic GdNi adopts a CrB type of crystal structure (space group Cmcm), and it orders ferromagnetically via a second-order phase transition at 70 K, exhibiting unusually strong spontaneous striction along the three independent crystallographic axes in the ferromagnetically ordered state. Here we introduce a microscopic model to describe anisotropic changes of lattice parameters and elastic contribution to magnetocaloric effect of GdNi. In the model, results of density functional theory (DFT) calculations are used as inputs into a Hamiltonian that includes elastic energy of an anisotropic crystal lattice, exchange interactions, and Zeeman effect. The magnetic and elastic Hamiltonians are coupled throughmore » an anisotropic Bean-Rodbell model of magnetoelastic interactions. This coupling gives rise to anisotropic changes in the lattice parameters observed experimentally, and the model reveals good to reasonable agreements between the current theoretical results and earlier experimental data, thus validating the model within the limits of assumptions made. We also show that DFT calculations with 4f electrons of Gd treated as core electrons lead to a more adequate estimate of elastic constants of GdNi in comparison with the LDA + U method where 4f electrons are treated as valence electrons.« less
  5. Origins of magnetic memory and strong exchange bias bordering magnetic compensation in mixed-lanthanide systems

    Here, the unexpected physical phenomena resulting from the seemingly inconsequential substitutions of chemically similar lanthanide elements in the Pr1-x GdxScGe system are exploited to further the understanding of rare-earth magnetism and inform materials design. By directly probing magnetic moments of crystallographically indistinguishable Pr and Gd we solve the puzzles of how an unusual magnetic memory and strong exchange bias emerge at specific, easily predictable chemistries. Both effects are rooted in a robust antiparallel arrangement of large 4f magnetic moments of light and heavy lanthanides. This enables precise control of nearly zero net magnetization either opposed to, or aligned with, themore » external magnetic field that persists over a wide range of temperatures and fields. Further, spontaneous perturbations in the random distribution of lanthanide ions makes strong exchange bias possible in bulk single-phase compounds bordering magnetic compensation, consequently expanding the materials base beyond artificial magnetic multilayers and broadening the range of potential applications of the phenomenon.« less
  6. Anomalous electrical transport behavior in the vicinity of the first-order magnetostructural transition in the giant magnetocaloric Gd4ScGe4

    Here, magnetic, specific heat, and electrical transport measurements of Gd4ScGe4 single crystals reveal sharp, discontinuous, nearly anhysteretic first-order magnetostructural transformation at $$T_C$$ = 63 K. The electrical resistivity exhibits two distinct regions where it increases with decreasing temperature: between $$T_C$$ and 120 K, as well as below 3 K; electronic transport remains conventionally metallic at all other measured temperatures, up to 325 K. The dispersion of charge carriers due to electron-paramagnon scattering is the likely reason for the observed anomalous transport above $$T_C$$. Additionally, the existence of intermediate lattice states near the transition recognized by the spike in the interslabmore » Ge-Ge distances is expected to reduce the mean free path of the electrons contributing to the unusual behavior of the electrical resistivity between $$T_C$$ and 120 K. Beyond conventional electronic and lattice terms, the third component of likely magnetic origin contributes to the low-temperature heat capacity; the presence of spin waves may be responsible for the increased electron-magnon scattering below 3 K. Minor magnetocrystalline anisotropy is observed with the b axis as the easy magnetization axis in Gd4ScGe4. A negative deviation from linearity in the temperature dependence of the inverse magnetic susceptibility is detected below 150 K.« less
  7. Inducing Fe moment in LaFeSi with p-block element substitution

    We studied the LaFeSi phase using density functional theory based full-potential linearized augmented plane wave (FP-LAPW) method. Specifically we examined the effect of p-element substitution on the stability and magnetic properties focusing on pathways to induce Fe magnetic moments. We demonstrate that either partial or complete substitutions at the Si 2 c-site by several p-block elements lead to non-zero Fe moments. Our theoretical study shows that partially substituted LaFeSi 1-y Ga y and LaFeSi 1-y Al y are more thermodynamically stable than the fully substituted LaFeGa and LaFeAl. We also found that the P substitutions, either partial or complete, havemore » the most negative formation energies, however the compounds containing phosphorus are non-magnetic. Our work highlights a pathway toward manipulations of the otherwise quenched Fe-moments in LaFeSi-related compounds and help in advancing the potential magnetic functionalities of LaFeX compounds.« less
  8. Correlating Crystallography, Magnetism, and Electronic Structure Across Anhysteretic First-Order Phase Transition in Pr2In

    Here, temperature-dependent powder X-ray diffraction and magnetization measurements of Pr2In conclusively prove that the unusual anhysteretic first-order paramagnetic-ferromagnetic phase transition in the compound is related to concurrent changes in both the magnetic and crystallographic lattices. At the same time, the hexagonal Ni2In-type structure is stable at least between 6 and 298 K, including at TC = ~57 K. From the density functional theory calculations, the electronic structure of the compound is extraordinarily sensitive to minor changes in lattice parameters that occur across the phase transition, revealing the origin of strong magnetoelastic coupling. In the vicinity of TC, the maximum entropymore » change, ΔSMax = -16 J Kg-1K-1 induced by a moderate magnetic field change of 20 kOe (ΔSMax = -20 J Kg-1K-1 for 50 kOe magnetic field change) is comparable to other known potentially functional materials demonstrating large cryogenic magnetocaloric effect.« less
  9. Toward efficient elastocaloric systems: Predicting material thermal properties with high fidelity

    A critical need to accurately model thermal behaviors of materials that exhibit strong elastocaloric effects, including predicting the effects themselves at varying stresses and temperatures, has been addressed using a simple and versatile physics-based approach. The key factor leading to the high precision is approximating the underlying elastic phase transition as a smooth modification of lattice entropy between coexisting phases. Once the phase transformation entropy is modeled to match experimentally measured strain as a function of temperature and applied stress, estimating the heat capacity, entropy, and isothermal entropy and adiabatic temperature changes in temperature-stress coordinates becomes straightforward. This approach providesmore » insight into how thermal properties of elastocaloric materials vary through the transition based on strain measurements that are simple to perform and interpret. In addition to aiding in the rapid evaluation of new and existing elastocaloric materials, this advance is expected to prove invaluable for accurate heat transfer modeling aimed at designing efficient regenerative elastocaloric cooling devices.« less
  10. Extraordinarily strong magneto-responsiveness in phase-separated LaFe2Si

    Materials responding vigorously to minor variations of external stimuli with negligible hysteresis could revolutionize many of the energy technologies, including refrigeration, actuation, and sensing. Here, 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,more » 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.« less
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