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Taking advantage of recent progress in neutron instrumentation and in the understanding of magnetic-field-dependent small-angle neutron scattering, here, we study the three-dimensional magnetization distribution within an isotropic Nd-Fe-B bulk magnet. The magnetic neutron scattering cross section of this system features the so-called spike anisotropy, which points towards the presence of a strong magnetodipolar interaction. This experimental result combined with a damped oscillatory behavior of the corresponding correlation function and recent micromagnetic simulation results on spherical nanoparticles suggest an interpretation of the neutron data in terms of vortex-like flux-closure patterns. The field-dependent correlation length Lc is well reproduced by a phenomenological power-law model. While the experimental neutron data for Lc are described by an exponent close to unity (p = 0.86), the simulation results yield p = 1.70, posing a challenge to theory to include vortex-vortex interaction effects., Comment: 16 pages, 5 figures

We employ micromagnetic simulations to model the effect of pore-type microstructural defects on the magnetic small-angle neutron scattering cross section and the related pair-distance distribution function of spherical magnetic nanoparticles. Our expression for the magnetic energy takes into account the isotropic exchange interaction, the magnetocrystalline anisotropy, the dipolar interaction, and an externally applied magnetic field. The signatures of the defects and the role of the dipolar energy are highlighted and the effect of a particle-size distribution is studied. The results serve as a guideline to the experimentalist., Comment: arXiv admin note: text overlap with arXiv:2205.07552

Magnetic nanoparticles offer unique potential for various technological, biomedical, or environmental applications thanks to the size-, shape- and material-dependent tunability of their magnetic properties. To optimize particles for a specific application, it is crucial to interrelate their performance with their structural and magnetic properties. This review presents the advantages of small-angle X-ray and neutron scattering techniques for achieving a detailed multiscale characterization of magnetic nanoparticles and their ensembles in a mesoscopic size range from 1 to a few hundred nanometers with nanometer resolution. Both X-rays and neutrons allow the ensemble-averaged determination of structural properties, such as particle morphology or particle arrangement in multilayers and 3D assemblies. Additionally, the magnetic scattering contributions enable retrieving the internal magnetization profile of the nanoparticles as well as the inter-particle moment correlations caused by interactions within dense assemblies. Most measurements are used to determine the time-averaged ensemble properties, in addition advanced small-angle scattering techniques exist that allow accessing particle and spin dynamics on various timescales. In this review, we focus on conventional small-angle X-ray and neutron scattering (SAXS and SANS), X-ray and neutron reflectometry, gracing-incidence SAXS and SANS, X-ray resonant magnetic scattering, and neutron spin-echo spectroscopy techniques. For each technique, we provide a general overview, present the latest scientific results, and discuss its strengths as well as sample requirements. Finally, we give our perspectives on how future small-angle scattering experiments, especially in combination with micromagnetic simulations, could help to optimize the performance of magnetic nanoparticles for specific applications., Comment: 34 pages, 16 figures

We employ magnetic small-angle neutron scattering to investigate the magnetic interactions in $(Fe_{0.7}Ni_{0.3})_{86}B_{14}$ alloy, a HiB-NANOPERM-type soft magnetic nanocrystalline material, which exhibits an ultrafine microstructure with an average grain size below 10 nm. The neutron data reveal a significant spin-misalignment scattering, which is mainly related to the jump of the longitudinal magnetization at internal particle-matrix interfaces. The field dependence of the neutron data can be well described by the micromagnetic small-angle neutron scattering theory. In particular, the theory explains the 'clover-leaf-type' angular anisotropy observed in the purely magnetic neutron scattering cross section. The presented neutron-data analysis also provides access to the magnetic interaction parameters, such as the exchange-stiffness constant, which plays a crucial role towards the optimization of the magnetic softness of Fe-based nanocrystalline materials., Comment: 13 pages,6 figures, 1 table, 1 footnote

Magnetic-field-dependent unpolarized small-angle neutron scattering (SANS) experiments demonstrate that high-pressure torsion (HPT) straining induces spin misalignments in pure Ni, which persist in magnetic fields up to 4 T. The spin-misalignment scattering patterns are elongated perpendicular to the applied magnetic field due to an unusual predominant longitudinal $sin^2(\theta)$-type angular anisotropy. Such a contribution cannot be explained by the conventional second order (in spin misalignment amplitude) micromagnetic SANS theory in the approach-to-saturation regime, nor can its magnitude relative to the other features of the cross sections by the third order micromagnetic SANS theory. This indicates that the high-density of crystal defects induced via HPT straining in Ni makes such higher-order effects in the micromagnetic SANS cross sections observable., Comment: 9 figures

We report the results of an unpolarized small-angle neutron scattering (SANS) study on Mn-Bi-based rare-earth-free permanent magnets. The magnetic SANS cross section is dominated by long-wavelength transversal magnetization fluctuations and has been analyzed in terms of the Guinier-Porod model and the distance distribution function. This provides the radius of gyration which, in the remanent state, ranges between about $220-240 \, \mathrm{nm}$ for the three different alloy compositions investigated. Moreover, computation of the distance distribution function in conjunction with results for the so-called $s$-parameter obtained from the Guinier-Porod model indicate that the magnetic scattering of a Mn$_{45}$Bi$_{55}$ sample has its origin in slightly shape-anisotropic structures.

We combine magnetometry and magnetic small-angle neutron scattering to study the influence of the microstructure on the macroscopic magnetic properties of a nanocrystalline Ni bulk sample, which was prepared by straining via high-pressure torsion. As seen by magnetometry, the mechanical deformation leads to a significant increase of the coercivity compared to nondeformed polycrystalline Ni. The neutron data reveal a significant spin-misalignment scattering caused by the high density of crystal defects inside the sample, which were created by the severe plastic deformation during the sample preparation. The corresponding magnetic correlation length, which characterizes the spatial magnetization fluctuations in real space, indicates an average defect size of 11 nm, which is smaller than the average crystallite size of 60 nm. In the remanent state, the strain fields around the defects cause spin disorder in the surrounding ferromagnetic bulk, with a penetration depth of around 22 nm. The range and amplitude of the disorder is systematically suppressed by an increasing external magnetic field. Our findings are supported and illustrated by micromagnetic simulations, which, for the particular case of nonmagnetic defects (holes) embedded in a ferromagnetic Ni phase, further highlight the role of localized spin perturbations for the magnetic microstructure of defect-rich magnets such as high-pressure torsion materials., Comment: This is the version of the article accepted for publication in Physical Review Materials including all changes made as a result of the peer review process, and which may also include the addition to the article by APS of a header, an article ID, a cover sheet and/or an Accepted Manuscript watermark, but excluding any other editing, typesetting or other changes made by APS and/or its licensors

Magnetic nanoparticles offer a unique potential for various biomedical applications, but prior to commercial usage a standardized characterization of their structural and magnetic properties is required. For a thorough characterization, the combination of conventional magnetometry and advanced scattering techniques has shown great potential. In the present work, we characterize a powder sample of high-quality iron oxide nanoparticles that are surrounded with a homogeneous thick silica shell by DC magnetometry and magnetic small-angle neutron scattering (SANS). To retrieve the particle parameters such as their size distribution and saturation magnetization from the data, we apply standard model fits of individual data sets as well as global fits of multiple curves, including a combination of the magnetometry and SANS measurements. We show that by combining a standard least-squares fit with a subsequent Bayesian approach for the data refinement, the probability distributions of the model parameters and their cross correlations can be readily extracted, which enables a direct visual feedback regarding the quality of the fit. This prevents an overfitting of data in case of highly correlated parameters and renders the Bayesian method as an ideal component for a standardized data analysis of magnetic nanoparticle samples., Comment: This is the version of the article accepted for publication in Nanotechnology including all changes made as a result of the peer review process, and which may also include the addition to the article by IOP of a header, an article ID, a cover sheet and/or an Accepted Manuscript watermark, but excluding any other editing, typesetting or other changes made by IOP and/or its licensors

We investigated a polycrystalline sample of the ferrimagnetic compound $\mathrm{Tb_{0.15}Co_{0.85}}$ by magnetometry and small-angle neutron scattering (SANS). The magnetization curve at 300 K is characteristic for soft ferrimagnets but at 5 K the hysteresis indicates the existence of magnetic domains. The magnetic SANS signal suggests that at 300 K the Tb and Co moments are correlated over large volumes within the micrometer-sized grains with correlation lengths > 100 nm. At 5 K, however, the magnetic SANS analysis reveals a reduced correlation length of around 4.5 nm, which indicates the formation of narrow magnetic domains within the ferrimagnet with one dimension being in the nm range. We attribute the observed changes of the domain structure to the temperature-dependence of the magnetic properties of the Tb sublattice., Comment: This is the version of the article accepted for publication including all changes made as a result of the peer review process, as submitted to Journal of Physics D: Applied Physics. IOP Publishing Ltd is not responsible for any errors or omissions in this version of the manuscript or any version derived from it. The Version of Record is available online at doi.org/10.1088/1361-6463/ab8b95

One of the key challenges in magnetism remains the determination of the nanoscopic magnetization profile within the volume of thick samples, such as permanent ferromagnets. Thanks to the large penetration depth of neutrons, magnetic small-angle neutron scattering (SANS) is a powerful technique to characterize bulk samples. The major challenge regarding magnetic SANS is accessing the real-space magnetization vector field from the reciprocal scattering data. In this letter, a fast iterative algorithm is introduced that allows one to extract the underlying two-dimensional magnetic correlation functions from the scattering patterns. This approach is used here to analyze the magnetic microstructure of Nanoperm, a nanocrystalline alloy which is widely used in power electronics due to its extraordinary soft magnetic properties. It can be shown that the computed correlation functions clearly reflect the projection of the three-dimensional magnetization vector field onto the detector plane, which demonstrates that the used methodology can be applied to probe directly spin-textures within bulk samples with nanometer-resolution., Comment: 9 pages, 3 figures

In the quest to image the three-dimensional magnetization structure we show that the technique of magnetic small-angle neutron scattering (SANS) is highly sensitive to the details of the internal spin structure of nanoparticles. By combining SANS with numerical micromagnetic computations we study the transition from single-domain to multi-domain behavior in nanoparticles and its implications for the ensuing magnetic SANS cross section. Above the critical single-domain size we find that the cross section and the related correlation function cannot be described anymore with the uniform particle model, resulting e.g. in deviations from the well-known Guinier law. We identify a clear signature for the occurrence of a vortex-like spin structure at remanence. The micromagnetic approach to magnetic SANS bears great potential for future investigations, since it provides fundamental insights into the mesoscale magnetization profile of nanoparticles., Comment: 6 pages, 3 figures

We report the results of an unpolarized small-angle neutron scattering (SANS) study on Mn-Zn ferrite (MZFO) magnetic nanoparticles with the aim to elucidate the interplay between their particle size and the magnetization configuration. We study different samples of single-crystalline MZFO nanoparticles with average diameters ranging between 8 to 80 nm, and demonstrate that the smallest particles are homogeneously magnetized. However, with increasing nanoparticle size, we observe the transition from a uniform to a nonuniform magnetization state. Field-dependent results for the correlation function confirm that the internal spin disorder is suppressed with increasing field strength. The experimental SANS data are supported by the results of micromagnetic simulations, which confirm an increasing inhomogeneity of the magnetization profile of the nanoparticle with increasing size. The results presented demonstrate the unique ability of SANS to detect even very small deviations of the magnetization state from the homogeneous one., Comment: 20 pages, 13 figures

Shell ferromagnetism is a new functional property of certain Heusler alloys which has been recently observed in $\mathrm{Ni}_{50}\mathrm{Mn}_{45}\mathrm{In}_{5}$. We report the results of a comparative study of the magnetic microstructure of bulk $\mathrm{Ni}_{50}\mathrm{Mn}_{45}\mathrm{In}_{5}$ Heusler alloys using magnetometry, synchrotron x-ray diffraction, and magnetic small-angle neutron scattering (SANS). By combining unpolarized and spin-polarized SANS (POLARIS) we demonstrate that a number of important conclusions regarding the mesoscopic spin structure can be made. In particular, the analysis of the magnetic neutron data suggests that nanoprecipitates with an effective ferromagnetic component form in an antiferromagnetic matrix on field annealing at $700 \, \mathrm{K}$. These particles represent sources of perturbation, which seem to give rise to magnetically disordered regions in the vicinity of the particle-matrix interface. Analysis of the spin-flip SANS cross section via the computation of the correlation function yields a value of $\sim 55 \, \mathrm{nm}$ for the particle size and $\sim 20 \, \mathrm{nm}$ for the size of the spin-canted region., Comment: 11 pages, 8 figures

The antisymmetric Dzyaloshinskii-Moriya interaction (DMI) plays a decisive role for the stabilization and control of chirality of skyrmion textures in various magnetic systems exhibiting a noncentrosymmetric crystal structure. A less studied aspect of the DMI is that this interaction is believed to be operative in the vicinity of lattice imperfections in crystalline magnetic materials, due to the local structural inversion symmetry breaking. If this scenario leads to an effect of sizable magnitude, it implies that the DMI introduces chirality into a very large class of magnetic materials---defect-rich systems such as polycrystalline magnets. Here, we show experimentally that the microstructural-defect-induced DMI gives rise to a polarization-dependent asymmetric term in the small-angle neutron scattering (SANS) cross section of polycrystalline ferromagnets with a centrosymmetric crystal structure. The results are supported by theoretical predictions using the continuum theory of micromagnetics. This effect, conjectured already by Arrott in 1963, is demonstrated for nanocrystalline terbium and holmium (with a large grain-boundary density), and for mechanically-deformed microcrystalline cobalt (with a large dislocation density). Analysis of the scattering asymmetry allows one to determine the defect-induced DMI constant, $D = 0.45 \pm 0.07 \, \mathrm{mJ/m^2}$ for Tb at $100 \, \mathrm{K}$. Our study proves the generic relevance of the DMI for the magnetic microstructure of defect-rich ferromagnets with vanishing intrinsic DMI. Polarized SANS is decisive for disclosing the signature of the defect-induced DMI, which is related to the unique dependence of the polarized SANS cross section on the chiral interactions. The findings open up the way to study defect-induced skyrmionic magnetization textures in disordered materials.