The ability of certain magnetic materials to change their entropy and/or temperature with the application and removal of a magnetic field (magnetocaloric effect, MCE) is a physical phenomenon that could lead to the realization of clean, energy-efficient heat pumping systems. We report a series of LaFe11.8Si1.1X0.1 compounds, where X = Al, Ga, and In, added in small concentrations, substantially reduce brittleness intrinsic to unsubstituted La(Fe1-xSix)13, while preserving or enhancing their giant MCEs [1]. Room temperature powder X-ray diffraction confirms formation of LaFe11.8Si1.1X0.1 adopting the NaZn13-type structure as major phases, with ~10 to 15% of Î±Fe impurity. Surprisingly, relatively large amounts of Î±Fe do not deteriorate the magnetic field-induced entropy change (Î”S), yet the resultant alloys have much improved mechanical stability. The corresponding maximum Î”S are -18, -17, and -13 J kg-1 K-1 for X = In, Al, and Ga, respectively, in Î”H = 2 T in the vicinities of their respective Curie temperatures. The Curie temperatures of LaFe11.8Si1.1X0.1 materials can be increased to room temperature and above by hydrogenation, preserving the giant MCE. For example, a fully hydrogenated LaFe11.8Si1.1In0.1H2.3 exhibits maximum Î”S close to -16 J kg-1 K-1 at T~344 K and Î”H =2 T. This work was supported by the Division of Materials Science and Engineering of the Office of Basic Energy Sciences of the U.S. DOE. Ames Laboratory is operated for the U.S. Department of Energy (DOE) by Iowa State University under Contract No. DE-AC02-07CH11358. AKP acknowledges the finanacial support from faculty startup fund from the Deanâ€™s Office, School of Arts and Sciences, SUNY Buffalo State.

Tailoring mechanical properties and magnetocaloric effect in LaFe11.8Si1.2 zXzHy (X = Al, Ga, In)

Kagome-lattice magnets RMn6Sn6 recently emerged as a new platform to exploit the interplay between magnetism and topological electronic states [1]. Some of the most exciting features of this family are the dramatic dependence of the easy magnetization direction on the rare-earth specie, despite other magnetic and electronic properties being essentially unchanged, and the Kagome geometry of the Mn planes that in principle can generate flat bands and Dirac points; gapping of the Dirac points by spin-orbit coupling has been suggested recently to be responsible for the observed anomalous Hall response in the member TbMn6Sn6. In this work [2], we address both issues with density functional calculations and are able to explain, with full quantitative agreement, the evolution of magnetic anisotropy, including a complete reversal upon adding an $f$-electron with zero magnetic orbital quantum number when going from Ho to Er. We also show the microscopic origin of this computational result using a simple and physically transparent analytical model. We analyze in detail the topological properties of Mn-dominated bands and demonstrate how they emerge from the multiorbital planar Kagome model. We further show that, despite this fact, most of the topological features at the Brillouin zone corner K are strongly 3D, and therefore cannot explain the observed quasi-2D AHE, while those few that show a quasi-2D dispersion are too far removed from the Fermi level. We conclude that, contrary to previous claims, Kagome-derived topological band features bear little relevance to transport in RMn6Sn6, albeit they may possibly be brought to focus by electron or hole doping. 
**References:** [1] J.-X. Yin, S. S. Zhang, H. Li, K. Jiang, G. Chang, B. Zhang, B. Lian, C. Xiang, I. Belopolski, H. Zheng, T. A. Cochran, S.-Y. Xu, G. Bian, K. Liu, T.-R. Chang, H. Lin, Z.-Y. Lu, Z. Wang, S. Jia, W. Wang, and M. Z. Hasan, Giant and anisotropic many-body spin-orbit tunability in a strongly correlated kagome magnet, Nature 562, 91 (2018) 
[2] Y. Lee, R. Skomski, X. Wang, P. P. Orth, A. K. Pathak, B. N. Harmon, R. J. McQueeney, I. I. Mazin, and L. Ke, Interplay between magnetism and band topology in Kagome magnets RMn6Sn6, arXiv 2201, 11265 (2022), https://arxiv.org/abs/2201.11265 

![](https://s3.eu-west-1.amazonaws.com/underline.prod/uploads/markdown_image/1/image/0f783c20cf93a9b8838fc51289261234.png) 
Fig. 1 Variation of magnetic energy (in meV/f.u.) as a function of spin-axis rotation in RMn6Sn6, with R = Gd, Tb, Dy, Ho, and Er, calculated (a) with and (b) without R-4f contributions. $\theta$ is the angle between the spin direction and the out-of-plane direction. The experimental easy directions for each compound are denoted by arrows in panel (a). The lines are just guides for the eye. 
![](https://s3.eu-west-1.amazonaws.com/underline.prod/uploads/markdown_image/1/image/6b36d3bf48826bb00709ef58034f99e5.png) 
Fig. 2 Band structures projected on surface BZ calculated without (blue) and with (red) SOC in TbMn6Sn6. The k-dependent DOS are integrated along kz and are calculated in DFT.

Interplay between magnetism and band topology in Kagome magnets RMn6Sn6

Considering the natural abundance of the constituting elements and first-order phase transition (FOPT), LaFe13-xSix-derived compounds have been extensively studied for magnetocaloric effect, a phenomenon that causes the cooling or heating of material when placed in an external magnetic field [1]. They are, however, extremely brittle and mechanically friable, showing rather low thermal conductivities and measurable irreversibility, which thus far could not be eliminated completely. Recently, Pathak et al. [2] reported the first-time discovery of a two-phase, naturally formed at the LaFe2Si stoichiometry rather than LaFe13-xSix compound. LaFe2Si exhibits strongly responsive behaviors without the degradation in properties that can be exploited in weak magnetic fields. However, the phase transition happens rather at low temperatures and the saturation moment is low. We are working on this material to further enhance the phase transition temperature and also to improve the magnetic and mechanical properties of the alloy. In this presentation, we will present the synthesis and characterization of LaFe2-yCoySi. We prepared LaFe2-yCoySi by making the first pre-alloy of FeCoSi and then added Co and melted several times. The alloys were further homogenized by the vacuum suction casting technique, which prepared a 4 to 5 cm long rod with a 6mm diameter of sample. The ferromagnetic to paramagnetic transition temperature increases from 199K for x = 0 to 273K for x = 0.3 and the full width at the half-maximum value of magnetic entropy changes increases significantly with Co doping. We discuss the phase transition, electrical transport, magnetic and magnetocaloric properties of LaFe2-yCoySi compounds.

Phase transition, electrical transport and magnetic entropy change of LaFe2 yCoySi alloys prepared by suction casting

Owing to the relative abundance of its constituent elements and large MCE observed near room temperature, the AlFe2B2 system has attracted much attention recently [1]. As an alternative to current rare earth materials, AlFe2B2 promises the realization of cleaner, energy efficient refrigeration technologies based on phenomena associated with MCE [2]. Additionally, excess Al is believed to generate phase impurities which can change the observed MCE properties of this system [3]. By dissolving certain impurities in acid, a significant enhancement of the MCE properties of this system have been observed [4]. Considering this behavior, we have studied the effect of acid treatment on the magnetic, magnetocaloric, and transport properties of Al0.85+xSi0.15Fe2B2 (x = 0.2, 0.4). The goal was to explore the possibility of enhancing the MCE properties of the materials by adding excess aluminum and subjecting them to acid treatment after annealing. The samples were prepared by arc melting followed by drop-casting. The drop-casted samples were annealed followed by acid treatment. The alloys were characterized by x-ray diffraction, scanning electron microscopy, dc magnetization, and electrical resistivity measurements. The second order ferromagnetic phase transitions were observed near room temperature (~298 K â€“ 315 K) and peak magnetic entropy changes (-Î”SM) of more than 4 J/kg K were observed for a field change of 5 T. The details of phase purity, microstructure, magnetic, and transport properties of the acid treated and the drop casted annealed materials will be presented.

The effect of acid treatment on the magnetic and magnetocaloric properties of Al rich Al0.85+xSi0.15Fe2B2

Magnetic refrigeration is an environmentally friendly cooling technology, which is believed to be significantly more efficient than the currently employed gas-compression-based cooling technologies. The commercialization of this technology is crucially dependent on the discovery of materials that exhibit large magnetocaloric effects and can be easily fabricated using cheap, non-toxic, and readily available elements. The intermetallic Mn1-xFex-Î´NiÎ´Si1-yAly compounds are known to exhibit large magnetocaloric effects at the relatively low magnetic field (H = 2T or lower) and tunable phase transition [1, 2]. These materials have gained much interest in recent years due to the fact that the constituent elements are cheap and readily available. However, selected drawbacks including large thermal hysteresis and mechanical instability make these materials unsuitable for application. More research efforts are required to eliminate these drawbacks so that the application potential for these materials can be realized. Therefore, we have synthesized the substitution of Ni with Co in Mn0.5Fe0.5Ni1-xCoxSi0.94Al0.06 (0.025 â‰¤ x â‰¤ 0.075) alloys by arc melting followed by a rapidly quenched vacuum suction casting technique and study the magnetic and magnetocaloric properties of the system, which has not been reported yet. X-ray diffraction and scanning electron microscopy (SEM) data indicated that the samples exhibited a single-phase. Peak magnetic entropy changes of (â€“ Î”SM) of as-cast alloy with x =0.025 is found to be 12 and 31 J kg-1K-1 for Î”H = 2 and 5 T, respectively around 225 K. The observed large MCEs are due to the first order magneto-structural phase transition exhibited by the materials from low-temperature ferromagnetic orthorhombic phase to high-temperature paramagnetic hexagonal phase. In this presentation, we present details of phase purity, microstructure, and magnetic properties of as-prepared and heat-treated alloys with 0.025 â‰¤ x â‰¤ 0.075

Magnetocaloric properties of Co doped Mn0.5Fe0.5Ni1

The MnTX (T = Ni, Co; X = p-block elements) compounds have received considerable attention due to the coupled first-order magnetic and structural phase transitions (MST) they exhibit. Large magnetocaloric effects are often associated with these phase transitions. The Mn1-xFexNiSi1-yAly system is a member of the MnTX family for which a large magnetic entropy change of 23 J kg-1 K-1 has been reported at T= 210K, ΔH = 2T. This value was reported for x = 0.5, y = 0.07 and for x = 0.5, y = 0.05 the peak value decreased to 17 J kg-1 K-1 (T = 315K, ΔH = 2T) (Biswas et. al. Acta Mat. 180 (2019) 341). For x = 0.4, y = 0.7, a peak magnetic entropy change of 9.3 J kg-1 K-1 was recently observed near 247 K (Ghosh et. al. JMMM 500 (2020) 166345). These studies suggested that the Mn1-xFexNiSi1-yAly system exhibits the maximum entropy change for x = 0.5. It is interesting to study the effect of Fe and Ni concentration variation on the magnetocaloric properties of the Mn0.5Fe0.5-xNi1-xSi1-yAly, which has not been reported yet. Therefore, in this work, we present an experimental study on the effects of partially replacing Fe with Ni on the structural, magnetic, and magnetocaloric properties of Mn0.5Fe0.5-xNi1+xSi0.94Al0.06 (0.025 ≤ x ≤ 0.10). The results of x-ray diffraction and scanning electron microscopy (SEM) showed that the samples exhibited a single-phase and energy dispersive spectroscopy analysis showed that the resulting compositions were close to the nominal compositions. Maximum magnetic entropy changes of – ΔSM = 22 and 57 J kg-1K-1 for ΔH = 2 and 5 T, respectively have been realized for x = 0.1 around 322 K. The observed large MCEs are due to the MST exhibited by the materials from low-temperature FM orthorhombic phase to high-temperature PM hexagonal phase. Work at SUNY, Buffalo State was supported by the startup fund from SUNY Buffalo State College and Undergraduate Summer Research Fellowship award, Undergraduate Research Office, Buffalo State.

The variation of Fe/Ni concentration and its effect on the magnetic and magnetocaloric properties of Mn0.5Fe0.5-xNi1+xSi0.94Al0.06

The LaFe13-xSix compounds have been studied for nearly two decades for their potential to serve as materials for magnetocaloric cooling. They exhibit either first- or second-order phase transitions depending on x(Si). Here we present the discovery of a naturally formed two-phase composite at the LaFe2Si stoichiometry, which exhibits strongly responsive behaviors without mechanical degradation that can be exploited in weak magnetic fields. Some of the unusual properties include a two-step, nearly anhysteretic first-order phase transformation between ferromagnetic (FM) and paramagnetic (PM) states, instead of a singular phase change present in conventional LaFe13-xSix, that is preserved in magnetic fields as high as 100 kOe. In addition to the giant magnetocaloric effect, the title material exhibits large, plateau-like positive magnetoresistance, both extending over a much wider temperature range when compared to phase-pure LaFe13-xSix. Finally, the composite also shows a Griffiths-like phase associated with short-range FM clustering in the PM state (Pathak et. al., Acta Mat. 215 (2021) 117083). We will also discuss the effect of impurities on magnetic, magnetocaloric, and transport behaviors of LaFe2Si. The work at Ames Laboratory was supported by the Division of Materials Science and Engineering, the Office of Basic Energy Sciences of the DOE. Ames Laboratory is operated for the U.S DOE by Iowa State University under Contract No. DE-AC02-07CH11358. Work at SUNY, Buffalo State was supported by the startup fund from SUNY Buffalo State College and the Undergraduate Research Office, Buffalo State.

Unusual magnetic, magnetocaloric, and transport properties in phase-separated LaFe2Si

A recent study shows that the magnetic entropy changes of Gd2O3 nanostructure depend on the morphology and it varies from - 8.7 J kg−1 K−1 for nanotubes to - 20 J kg−1 K−1 for the rod. Several attempts have been made to study the magnetocaloric effect (MCE) on different morphology but comparative study on morphology dependent MCE is missing. Here we investigate the MCE of Gd2O3 nanoparticles of different morphology. Single-phase Gd2O3 nanoparticles were synthesized via the hydrothermal method and a homogeneous precipitation method followed by heat-treated in the air at 1100OC for 12h. Four Gd2O3 nanoparticles of different shapes viz. bulk, rod, spheres, and plate were prepared. The morphology of the samples was analyzed using a scanning electron microscope (SEM). The SEM images of synthesized Gd2O3 showed fine 1D nano-rods, 2D nano-plates-like architecture prepared via hydrothermal method while hollow nanosphere morphology was achieved with a homogeneous precipitation method. The phase identification and lattice parameter of the powders were performed using x-ray diffraction which showed the presence of a highly crystalline single phase cubic crystal structure. Magnetic measurements were performed from 5 to 100K and magnetic field up to 50kOe. The material demonstrated typical paramagnetic behavior in the whole measured temperature region. The M-H data in the temperature range of 3–30 K is used to calculate the isothermal magnetic entropy change. The maximum value of ΔSm for 50 kOe field change at 5K is 11.2 J kg−1 K−1 for the nanoplate sample, 9.4 J kg−1 K−1 for the nano-rod, and 9.2 J kg−1 K−1 for the nano-sphere, and 10.7 J kg−1 K−1 for Bulk. The large ΔSm could be attributed to the surface area and surface geometry of the sample. More surface area indicates more surface spins that enhanced magnetization value. These results show the Gd2O3 nanoplates are promising materials for low-temperature application. Work at SUNY, Buffalo State was supported by the startup fund from SUNY Buffalo State College and the Undergraduate Research Office, Buffalo State.

Study the magnetocaloric properties of shape-dependent nanostructured Gd2O3: Nanoplates, Nanorods, and Nanospheres

Ternary RScGe intermetallics (R = Rare earth) crystallizing in a layered CeScSi-type structure (space group I4/mmm) demonstrate rich physics and a range of diverse magnetic phenomena. For example, PrScGe exhibits multiple magnetic transitions: paramagnetic (PM) to antiferromagnetic (AFM), then AFM to ferrimagnetic (FIM), and finally FiM-I to FiM-II upon cooling.1 GdScGe, in contrast, remains ferromagnetic below its Curie temperature (TC) of 350 K, which is notably higher than the TC (= 293 K) of its only magnetic constituent, Gd.2 These RScGe systems become even more interesting with substitutional alloying or additions of interstitials. Thus, Sm1-xNdxScGe shows an extraordinary large exchange bias3 and GdScGeH exhibits a loss of dimensionality and magnetic order.4 Here, through x-ray magnetic circular dichroism (XMCD) measurements, we report the interplay between Gd and Pr atoms in representatives of pseudo-ternary Pr1-xGdxScGe. We present direct evidence of antiparallel coupling between heavy and light lanthanide ions that occupy the same sublattice resulting in near zero magnetization. We explain how coupling magnetic compensation with small cooling fields can create magnetic memory – possibly opening up a new avenue for magneto-thermal memory devices. Lastly, we discuss the addition of hydrogen and its effects on dimensionality and electronic structure. This work was supported by the Office of Science of the U.S. Department of Energy (DOE), Division of Materials Sciences and Engineering, Office of Basic Energy Sciences. The Ames Laboratory is operated for the U.S. Department of Energy (DOE) by Iowa State University of Science and Technology under contract No. DE-AC02-07CH11358. XMCD research at the Advanced Photon Source was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Science, under contract DE-AC02-06CH11357.

Magnetic Interplay Between Gd and Pr in the CeScSi-type Layered Structure

Quantum phase transition (QPT) is a 2nd order solid state phase transition that starts at a quantum critical point (QCP) and continues to 0 K. Since all thermal fluctuations are absent at 0 K, QPT is caused by strong quantum fluctuations1. Since the lowest measuring temperature that can be experimentally reached in a research laboratory is between 20 mK and 50 mK, the QCP is generally determined by performing an extrapolation of the experimental data points (to 0 K) in the p vs. T (p is the control parameter and T is the temperature) phase diagram. ZrNi2Ga is a superconductor and belongs to the Ni-based Heusler family. The material exhibits a superconducting phase transition at ~2.9 K.2 When Ni is partially replaced by Cu in ZrNi2-xCuxGa the transition temperature linearly decreased to 1.85 K for x = 0.25.3 This is indicative of QPT in the system. Here, we have studied the magneto-transport properties of ZrNi2-xCuxGa (0.25 &lt; 0 ≤ 0.5) to further explore the possible QPT in the system. The samples were prepared by arc melting and the transport measurements were done on a Physical Property Measurement system with Helium-3 attachment. All samples exhibited the L21 cubic structure at room temperature. A superconducting phase transition temperature of as low as ~1 K was observed in the system, which nearly confirms the possibility of QPT in the ZrNi2-xCuxGa system. The experimental results will be presented in details.

Quantum Phase Transition in Partially Cu-Doped ZrNi2-xCuxGa Heusler Alloys

Ni2MnGa is an exemplary Heusler alloy to exhibit the martensitic phase transformation (MPT) from the high-temperature austenite phase to a lower temperature martensite phase.[1] The martensitic transformation occurs at TM ≈ 202 K followed by a ferromagnetic phase transition at TCA ≈ 380 K. When Mn is partially substituted by Cr in Ni2Mn1-xCrxGa TM increased while TC decreased, such that the two transitions overlapped at ~260 K for x = 0.50.[2] Additionally, the alloys exhibited resistivity drops of 2.5 - 18 % at the MPT. The largest magnitude drop occurred in materials exhibiting TM &gt; TC. Here, we present an experimental study on the transport and magnetic properties of Fe doped Ni2Mn0.4-xFexCr0.6Ga and Ni2Mn0.4FexCr0.6-xGa Heusler alloy systems. The goal was to compare the magnetic and transport properties of the two systems where Mn is replaced by Fe in one system and Cr is replaced by Fe in the other. All compounds were prepared by arc melting and annealing techniques. The samples were subjected to x-ray diffraction, electrical resistivity, and dc magnetization measurements. The diffraction data showed the samples were either tetragonal or Cubic at room temperature. For both systems TM and TC decreased with increasing x. However, TM decreased much rapidly for the Ni2Mn0.4FexCr0.6-xGa system while the rate of decrease of TC was slower. The experimental results will be presented and discussed taking the valence electron concentration, e/a, and the structural disorder into consideration.

A comparative study of the martensitic phase transitions in Fe doped Ni2Mn0.4-xFexCr0.6Ga and Ni2Mn0.4FexCr0.6-xGa Heusler alloy systems

The exchange bias (EB) phenomenon, generally quantified by the shift of the hysteresis loop along the magnetic field axis, has been observed in several Mn-rich Heusler alloys [1, 2, 3]. The fundamental science that drives EB and its technological impact are both of great interest [4, 5]. The EB effect in Mn-rich Heusler alloys is primarily related to the coexisting ferromagnetic (FM) and antiferromagnetic (AFM) interactions. Interestingly, the Mn atoms are responsible for both the FM and AFM interactions in these materials. In the Heusler alloy Mn(2)NiGa, both FM and AFM interactions are present. However, the material does not exhibit any EB effect. Interestingly, a strong EB was observed in Ga-deficient/Ni-rich Mn(2)Ni(1.4)Ga(0.6), which demonstrated the importance of crystalline site occupancies of the Mn atoms in driving EB [6]. Here, we have performed an experimental study on the effect of Fe doping on the magnetic and EB properties of Mn(2-x)Fe(x)Ni(1.6)Ga(0.4) (0 ≤ x ≤ 0.35). The goal of the study was to explore the effect of Fe doping on the FM and AFM interactions in the system. The samples were fabricated by arc melting, drop-casting, and annealing techniques. X-ray diffraction measurements and the scanning electron microscopy images showed that the alloys were phase segregated with two different lower symmetry structures. For all values of x, EB was observed in the materials. An EB field of as large as ~4000 Oe and a coercive field of ~14 kOe were observed in the materials. The structural, magnetic, and EB properties of all the alloys in the Mn(2.x)Fe(x)Ni(1.6)Ga(0.4) system will be presented.

The Magnetic and Exchange Bias Properties of Phase Segregated Mn2-xFexNi1.6Ga0.4

Mn0.5Fe0.5NiSi0.95Al0.05 is a member of the MnTX (T = Ni, Co; X = p-block elements) family of intermetallic compounds. It exhibits a first-order ferromagnetic transition coupled with a structural phase transition at 315 K. Near this transition a large magnetic entropy changes of ~17 J kg-1 K-1, for a field change of ΔH = 2 T, has been reported for Mn0.5Fe0.5NiSi0.95Al0.05.[1] In this work, we present an experimental study on the crystalline, magnetic, and magnetocaloric properties of Ni deficient (Mn-rich) Mn0.525Fe0.5Ni0.975Si0.95Al0.05. The study has been performed by x-ray diffraction, scanning electron microscopy, and dc magnetization measurements. X-ray diffraction measurements showed that the sample simultaneously exhibited the orthorhombic and hexagonal structures at room temperature. The ferromagnetic transition temperature occurred at ~338 K, which is significantly larger than 315 K observed in Mn0.5Fe0.5NiSi0.95Al0.05. A maximum magnetic entropy changes of ΔSM = -9.5 and 25 J kg-1K-1 for ΔH = 2 T and 5 T, respectively, has been observed. Reasonably large refrigeration capacity of 60 J /kg and 160 J/kg for field changes of ΔH = 2 T and 5 T, respectively, has also been observed. The experimental results and related discussions will be presented in detail. Work at SUNY, Buffalo State was supported by the startup fund from SUNY Buffalo State College and Undergraduate Summer Research Fellowship award, Undergraduate Research Office, Buffalo State.

Near room temperature magnetocaloric properties in Ni deficient Mn0.525Fe0.5Ni0.975Si0.95Al0.05

NOB: Magnetocaloric Materials I

technical paper

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KOA: Hard Magnetic Materials I: Rare Earth-based Compounds

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**Session Chair:** Radhika Barua, *Virginia Commonwealth University*

NPA: Magneto-Elastic, -Optical and Other Phenomena

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**Session Chair:** Arjun Pathak, *State University of New York, Buffalo State*

NPB: Magnetocaloric Materials III

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FOA - Magnetocalorics I

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Arjun Pathak

13

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