United States

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.

2022 Joint MMM-INTERMAG

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

The 15th Joint MMM-INTERMAG Conference (2022 Joint) is sponsored jointly by AIP Publishing and the IEEE Magnetics Society. Members of the international scientific and engineering communities interested in recent developments in fundamental and applied magnetism are invited to attend and contribute to the technical sessions. The technical program will include invited and contributed papers in oral and poster sessions, invited symposia, a plenary session, and an evening session, with about 1500 presentations overall. This Conference provides an outstanding opportunity for worldwide participants to meet their colleagues and collaborators and discuss developments in all areas of magnetism research.

The 2022 Joint Conference will offer both in-person and prerecorded on-demand content.

For tickets to the event, please register at the following link: https://magnetism.org/register

Please register for the Joint MMM-Intermag conference to join the event.

This Conference provides an outstanding opportunity for worldwide participants to meet their colleagues and collaborators and discuss developments in all areas of magnetism research.

poster

FePt nanoparticles (NPs) with fct (L10) structures have a wide promising application in high-density magnetic storage media, catalysis, and biomedicine [1, 2], because of their high magnetocrystalline anisotropy, catalytic activity, and good biocompatibility. Ag addition can promote ordering transition and directly obtain L10-FePt NPs with high structural ordering [3-5]. However, the ordering mechanism of the NPs by Ag addition and the ordering transition process are rarely reported. Herein, we report the direct synthesis of L10-FePt NPs by Ag addition. The ordering transition process was investigated, and the ordering mechanism was discussed. The metal precursors Pt(acac)2, Fe(acac)3, and AgAc were dissolved in HDA in the presence of HDD as reductant. And then the mixed solution was heated to 360 °C for 180 min. Finally, the product was collected by centrifugation with ethanol. The phase structure and magnetic properties of a series of products sampled at 360 °C for different reaction times (from 0 min to 180 min) are shown in Fig. 1 and Fig. 2, respectively. The precursors of Ag and Pt were firstly reduced, and form AgPt phase at beginning of the reaction. With reacting for 10 min, the precursor of Fe was reduced, and the FePt NPs were obtained. The products were mainly combined of elemental Ag and L10-FePt phases. The magnetic properties of the products changed from diamagnetic to ferromagnetic. With extending the reaction time, the both content of Ag and L10-FePt phases continuously increased. The coercivity of products enhanced from 0.9 kOe to 6.3 kOe with increasing the reaction time from 10 min to 180 min. These results indicate that Ag atoms are easy to migrate and enrich because of their low surface energy and high mobility. The Ag migration helps the formation of a large number of defects and vacancies in the crystal lattice, which can promote the rearrangement of atoms, and reduce the ordering transition barrier. Therefore, Ag addition can result into improvement of structural ordering of the FePt NPs.


![](https://assets.underline.io/uploads/markdown_image/1/image/81f76544f273f94ac19ed3a8359a5ab6.jpg)


Fig.1 The XRD patterns of products obtained at 360 °C for different reaction times

![](https://assets.underline.io/uploads/markdown_image/1/image/166d467e2867a3c4344affaf327827f5.jpg)


Fig. 2 The hysteresis loop of products obtained at 360 °C for different reaction times

Ordering Mechanism of L10-FePt Nanoparticles Synthesized by Ag Addition

Nanocomposite magnets composed of Nd2Fe14B and α-Fe nanoparticles are not only expected to increase the (BH)max compared to Nd-Fe-B magnets [1], but also effective in reducing the use of HREs [2]. Recently, we have reported on NdFeB/Mo/FeCo multilayered magnet films formed by a two-step method [3]. However, long-time multi-step annealing (MSA) using a halogen lamp was necessary to realize this magnet film. It is well known that method using a laser is an excellent technique that can significantly reduce the process time and is expected to improve the magnetic properties. In this study, we report the formation of nanocomposite NdFeB/Mo/FeCo magnet films using infrared laser annealing (iLA) technique. The Nanocomposite [NdFeB(30 nm)/Mo(0.3 nm)/FeCo(5 nm)/Mo(0.3 nm)]5 multilayered magnet films were prepared by UHV sputtering [3] followed by iLA processing. It is equipped with a CW semiconductor laser with a wave length of 939.8 nm and a spot size of about 5 mm in diameter on surface of films. Fig. 1 shows in-plane magnetization curves of the multilayered films as-deposited and iLA processed at 760°C. Both films with and w/o Mo interlayer before iLA processing showed soft magnetism with small coercivity and weak perpendicular magnetic anisotropy (PMA). The PMA of the film with the Mo interlayer is larger than that of the film without the Mo interlayer. Magnetic properties of both films were drastic changed from soft magnetism with PMA to hard magnetism with in-plane magnetic anisotropy after iLA processed at 760°C. Coercivity of in-plane of iLA processed film with Mo interlayer was 10 kOe which was double of the film w/o Mo interlayer. After iLA process, we can see that the squareness of film was improved by the introduction of Mo interlayer. These results show that the iLA process is effective in forming in-plane anisotropic nanocomposite NdFeB/Mo/FeCo magnet films even though the processing time of the iLA process is 1/100 of the processing time of the MSA process [3].


![](https://assets.underline.io/uploads/markdown_image/1/image/4abf4bd1b86901df35a7bb50f4fa6b41.jpg)


An in-plane magnetization curves of [Nd-Fe-B/Mo(tMo = 0 nm, 0.3 nm)/FeCo]5 multilayered films as-deposited state and iLA processed at 760°C.

Infrared Laser Annealing of Nanocomposite Nd-Fe-B/Mo/FeCo Multilayered Magnet Films

Effects of La3+ and Cu1+ co-doping on structural and magnetic properties of M-type strontium hexaferrite have been studied by using crystallographic and magnetic measurements. Stoichiometric Sr1-xLaxFe12-x/2Cux/2O19 (x=0, 0.25, 0.5, 0.65) samples have been prepared by the conventional ceramic method using La2O3, SrCO3, Fe2O3, and CuO powders with repeated sintering at 1300 °C for 24 hours. EDS analysis showed that the ratios of metal elements were in good agreement with compositions of the samples. XRD patterns showed that when x ≥ 0.7, LaFeO3, SrFeO3-δ, and CuFe2O4 coexisted along with the M-type hexaferrite. Lattice parameters deduced from the GSAS refinement shows that a slightly increases while c decreases with increasing x (Table 1). Variations of the saturation magnetization MS and the coercivity HC with x was obtained from room temperature VSM measurement as in Table 1. Whereas the HC decreases monotonically with x, the MS increases with the La3+ - Cu1+ co-doping throughout the doping range examined. Effective magnetic anisotropy constants K are calculated as well from the hysteresis curves using the law of approach to saturation method. K shows gradual increase with increasing x as listed in Table 1. XPS Cu2p scan shows that dominant valence state of Cu is +1. There were no trace observed for Cu2+ or metallic Cu (Fig. 1(a)). Apparently, monovalent Cu1+ has no spin magnetic moment. In view of the fact that diamagnetic substitution of either 4f1 or 4f2 site give rise to positive contribution to MS, this behavior strongly suggests that Cu1+ ions preferentially replace Fe3+ ions at those sites. Finally, Mössbauer spectra show gradual decrease in 4f2 intensity, in support of the octahedral 4f2 site preference of Cu1+. In addition, one extra sextet with Hhf ≈ 341 kOe was detected from the Mössbauer spectra, which were explained by the 12k site Fe3+ that have more than one 4f2 Cu1+ neighbors (Fig. 1(b)).

![](https://assets.underline.io/uploads/markdown_image/1/image/cd4821a42565474b6f0714cd6daacbb7.jpg)

Various parameters of Sr1-xLaxFe12-x/2Cux/2O19 (x=0, 0.25, 0.5, 0.65)


![](https://assets.underline.io/uploads/markdown_image/1/image/a24b2b3f1b09efbbee07fd50283fefb2.jpg)

(a) XPS Cu 2p scan for Sr0.5La0.5Fe11.75Cu0.25O19 and (b) room temperature Mössbauer spectra of Sr0.35La0.65Fe11.675Cu0.325O19

Structural, Magnetic, and Mössbauer Spectroscopic Study of La3+ and Cu1+ Co-doped M-type Strontium Hexaferrite

Exchange-coupled hard/soft ferrite nanoparticles are prospective to squeeze out a part of expensive magnets based on rare-earth elements. However, known exchange-coupled composite ferrite nanoparticles often suffer from a lack of a powerful enough hard-magnetic core, a high defectivity of magnetic phases, and a poor interface between them. Herein we demonstrate the first efficient synthesis of sandwiched nanomagnets, which exhibit the pronounced exchange-coupling effect. This work is featured by using individual high-coercive strontium hexaferrite nanoplates prepared by a borate glass crystallization method as cores for the composite particles. High crystal quality of the hexaferrite cores as a substrate provides an epitaxial growth of CoFe2O4 layers on the 001 facets from the organic high-boiling solvent and results in enhancing the remanence magnetization and the maximum energy product of the composite material. The obtained composite nanoparticles are characterized by well-defined epitaxial interfaces between the constituent phases. The exchange coupling results in strongly different magnetic properties compared to ones expected for a mechanical mixture of hexaferrite and cobalt ferrite. At room temperature, the magnetic properties are determined by the uniaxial magnetocrystalline anisotropy of the hexaferrite, while upon cooling the situation changes to the triaxial magnetocrystalline anisotropy typical for the spinel cobalt oxide. In the temperature range 5 – 300 K the composite shows significant improvement of the (BH)max values of both initial phases. The results of this work open new prospects for fabrication of multilayer oxide heterostructures with a synergetic performance which expands applications of exchange-coupled composites. The research was supported by Russian Science Foundation grant no 20-73-10129

Sandwiched CoFe2O4/SrFe11.5Al0.5O19/CoFe2O4 nanoparticles with exchange-coupling effect

Manipulations of micro-sized magnetic particles by an external field have been widely studied for the applications in MEMS and biofluidics. A popular way of manipulation is forming a microchain containing several particles in a liquid environment. The chain can be well controlled by a designated external field to perform rotation [1] or oscillation [2] for desired purposes. Nevertheless, the induced hydrodynamic drag would affect the formation and motion of the chain, such as the well studied chain rupture in a dynamic field. In the present paper, study of motion synchronicity of a micro-magnetic-particle chain in a rotating field is focused. To achieve synchronous rotation with the external field, force balance acting on the chain is required. Experiments are performed firstly to identify actual rotating frequency of an un-ruptured chain, denoted as fc, subjected to various field frequency fH. As the results shown in figure, for a 3-particle chain, motion synchronicity can only preserved up to a critical field frequency. Beyond this critical field frequency, the average rotating frequency of the chain starts to decay. The critical field frequency increases if magnetic field strength H is raised. The mechanism of this asynchronous motion can be understood by the competition of magnetic torque and hydrodynamic torque. The predicted critical frequencies, based on two approximations reported in the literatures [3,4], i.e., fc1 and fc2 shown in the figure, agree well with the experiments. In addition, temporal dynamical motion is also presented to illustrate the asynchronous motion.

![](https://assets.underline.io/uploads/markdown_image/1/image/fa77da4a4f02a4fcfe4bf92f2f888ada.jpg)

Actual rotating frequency of a 3-particle chains fc subjected to various field frequency fH. Marks of circle (O) and cross (X) are the predicted critical frequency for correspondent field strength H. The linear lines inductae synchronous motion of the chain and external field. Beyond a critical frequency, the actual rotating frqeuency of chain fc starts to drop. The predicted critical frquencies for different field strength H agree well with the experiments.

Motion Synchronicity of a Micro-magnetic-particle Chain in a Rotating Field

Magnetite is one of the oldest known magnetic materials. At room temperature, magnetite exhibits an inverse spinel structure with Fe3+ ions split between tetrahedral and octahedral sites, and Fe2+ ions occupying only octahedral sites. As it is well known, with decreasing temperature, magnetite undergoes a first order magnetic transition accompanied by a metal-insulator transition: the so-called Verwey transition (~120 K) [1]. However, there is another magnetic transition taking place at even lower temperatures (&lt; 50 K), whose underlaying nature is still not well understood. In bulk magnetite, a few studies have attributed this transition to different causes, such as the freezing of conduction electrons or rearrangement of electrons within domain walls [2,3]. Of particular interest is the case of magnetite nanoparticles, whose magnetic properties have been extensively studied in the last decades due to their multiple applications, especially in biomedicine [4]. However, a clear understanding on the presence of this transition in these nanoparticles has remained elusive [5]. Therefore, this work has been focused on the study of the low T transition in several types of magnetite nanoparticles, with different sizes, shapes, and purities. These nanoparticles have been structurally and morphologically characterized by using a combination of X-ray Diffraction and Transmission Electron Microscopy. Different oxidation states of the nanoparticles (i.e., into maghemite) have been revealed. Their magnetic response has been analyzed both as a function of the temperature (M vs. T, 5-300 K) and the magnetic field (M vs. H, up to 5 T). Some of these nanoparticles have exhibited a magnetic response close to the bulk, with saturation magnetization ~90 Am2/kg (300 K) and a clear Verwey transition. The low T transitions have been studied by AC susceptibility. In all cases, we have observed 1 or 2 magnetic transitions below 50 K, even for single domain nanoparticles. The nature of these transitions has been further investigated by using different spin relaxation models. Arrhenius law fittings suggest electron hopping freezing (τ0 = 10-8 – 10-9 s, and EB/kB = 200-300 K) for the nanoparticles with magnetic behavior closer to the bulk.

Magnetite Nanoparticles: A Detailed Analysis of the Low Temperature Magnetic Transitions

Over the past few years, the outstanding magnetic properties of highly crystalline iron oxide (Fe3O4) nanorods (NRs) have been extensively investigated by us for advanced magnetic hyperthermia [1], as well as spintronics applications [2]. Building upon this success, we propose an effective thermal treatment approach to creating a novel class of iron oxide core/shell structured nanorods. In this study, we demonstrate how Fe3O4/α-Fe2O3 core/shell structures can be formed in these nanorods through a controlled annealing process. The highly crystalline Fe3O4 nanorods were hydrothermally grown first and then annealed at 250° C for different periods of time (1, 3, 5, 7, and 9 h) to form Fe3O4/α-Fe2O3 core/shell structures, which are characterized by XRD and TEM. Magnetometry measurements indicate that the Verwey transition becomes sharper with increasing the annealing duration, which is attributed to the improved crystallinity of the Fe3O4 phase. Relative to the as-synthesized NRs, the saturation magnetization of the annealed NRs is reduced considerably, which is resulted from the reduced volume fraction of the Fe3O4 core and the formation of the antiferromagnetic α-Fe2O3 shell. When the annealing duration is extended to 5 h, a sharp drop in magnetization is observed in the temperature-dependent magnetization around 260 K which is associated with the Morin transition of the α-Fe2O3 layer. Interestingly, zero-field-cooled and field-cooled magnetic hysteresis loops show a negligible horizontal shift but a significantly large enhancement in magnetization was observed when the core/shell NRs are cooled down in a magnetic field of 1T from the room temperature, suggesting the presence of an intermediate layer composed of canted/disordered spins in between the core and shell. These findings indicate that the Fe3O4/α-Fe2O3 core/shell nanorods would be an excellent model system for probing interfacial magnetism at the nanoscale [3].

Coexistence of Verwey and Morin transitions and emerging magnetic phenomena in iron oxide core/shell nanorods

Multifunctional nanomaterials are an essential requirement to prepare smart sensor- or actuator-based devices [1]. Some of multifunctional materials can be found in the large group of Heusler alloys. Ni2FeGa and Ni2MnGa-based Heusler alloys are well known for their magnetocaloric and shape memory behavior [2], [3]. Moreover, their properties depend on the overall chemical composition, which makes them tunable [4]. Fabrication of magnetocaloric and shape memory Heusler alloys-based nanowires might be the next step to prepare a nanodimensional sensing and actuation device. Furthermore, these materials show a multifunctional behavior. It makes them suitable for preparation of a simultaneous sensing and actuation device. This research aims to describe the magnetocaloric and ferromagnetic shape memory behavior of electrochemically fabricated Heusler alloy-based nanowires with the chemical composition of Ni-Fe-Ga and Ni-Mn-Ga (Figure 1). Preparation of the Ni-Fe-Ga and Ni-Mn-Ga nanowires in an array introduces a magnetostatic interaction between the adjacent nanowires into the system. Combined with their shape anisotropy, it is possible to prepare nanowires with a highly efficient magnetocaloric behavior. The magnetic entropy change of &gt;0.2 J/kg.K was observed for the Ni-Fe-Ga nanowires (Figure 2). The Ni-Mn-Ga nanowires show an inverse magnetocaloric effect with the magnetic entropy change of even higher values. The magnetic field with the strength of up to 2 T was applied in the parallel direction with respect to the individual nanowires' longitudinal axes for both the Ni-Fe-Ga and Ni-Mn-Ga nanowires. Moreover, the structural transformation region associated with the magnetocaloric and shape memory processes of the Ni-Fe-Ga and Ni-Mn-Ga nanowires was observed above room temperature. Therefore, application of the prepared nanowires can be found in the temperature region of the human body or at the working temperatures of the majority of electrotechnical devices.

![](https://assets.underline.io/uploads/markdown_image/1/image/b29b34a7e23d9b52b1b711bb6310561a.jpg)

Fig.1: SEM micrograph of the electrochemically prepared Ni-Mn-Ga nanowires

![](https://assets.underline.io/uploads/markdown_image/1/image/5274a388b3f35e6f19e87abe71b08bd8.jpg)

Fig.2: Magnetic entropy change of the magnetocaloric Ni-Fe-Ga nanowires at different applied magnetic fields

Magnetocaloric Effect and Ferromagnetic Shape Memory Behavior of Electrodeposited Nanowires Array

As the number of biomedical applications of superparamagnetic iron-oxide nanoparticles (SPION) grows, having a detailed understanding of their magnetic state is increasingly important. It is commonly assumed that dipole-dipole interactions are not relevant for superparamagnetic nanoparticles because of thermal fluctuations. Here we show evidence that dipole-dipole interactions do indeed affect the collective magnetic state of a SPION sample. Ferromagnetic resonance spectroscopy of iron-oxide nanoparticles with a diameter of 10 nm reveals that the configuration of the particles has a strong effect on their effective magnetic anisotropy on short time scales. Fitting the experimental spectra using a theoretical model [1] enables the quantification of these anisotropy fields. Nanoparticles in suspension with a surfactant exhibit an easy-axis anisotropy due to field-induced alignment, whereas condensed dry nanoparticles (which no longer have the surfactant) exhibit an easy-plane anisotropy due to agglomeration. The difference between the effective uniaxial anisotropies in suspension versus the dry state is on the order of 0.1 T. The effective uniaxial anisotropies exhibited by the nanoparticles in these configurations are an order of magnitude larger than the intrinsic magneto-crystalline anisotropy. This suggests that dipole-dipole interactions can be important to the collective magnetic state of superparamagnetic systems despite thermal fluctuations and should be considered for high-frequency applications.

Ferromagnetic resonance of superparamagnetic iron-oxide nanoparticles: quantification of dipole-dipole interactions

The Ga2-xFexO3 (GFxO) compound, is a quite interesting material due to simultaneous exhibit magnetic and electric orderings [1,2]. However, the physical properties of GFxO at reduced grain sizes remain underexplored due to the challenges associated with their synthesis with a proper control over the crystalline phase. In addition, the effect of the Fe/Ga ratio on the magnetic properties of the nanosized GFxO system has not yet been completely established. In this work, therefore, we prepare a series of GFxO nanoparticles with 0.8 ≤ x ≤ 1.2 using the sol-gel method to systematically study the effect of the Fe/Ga ratio on their structural and magnetic properties. All the samples of GFxO with 0.8 ≤ x ≤ 1.2 have been characterized by the powder XRD measurements and Rietveld refinements. All the observed peaks can be indexed by reflections of the Pc21n orthorhombic structure of GFxO, and no impurity phase was found. The determined lattice parameters are found to display a monotonic increase with the Fe content x. Composition of the GFxO nanoparticles was confirmed by energy dispersive X-ray spectra. The evolution of the Néel temperature (TN) of GFxO samples versus their Fe-content (x). It is found that with increasing Fe-content, up to 1.2, the TN increases from 279 to 350 K. Moreover, the magnetic hysteresis curves measured below TN exhibit two-phase-like magnetic behavior consisting of soft and hard magnetic phases. The results could be explained by the site-disorder of the cations in GFxO nanoparticles.

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Ordering Mechanism of L10-FePt Nanoparticles Synthesized by Ag Addition

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