Magnetic nanoparticles (MNPs) have become increasingly important in biomedical applications like magnetic imaging and hyperthermia based cancer treatment. Understanding their magnetic spin configurations is important for optimizing these applications. The measured magnetization of MNPs can be significantly lower than bulk counterparts, often due to canted spins. This has previously been presumed to be a surface effect, where reduced exchange allows spins closest to the nanoparticle surface to deviate locally from collinear structures. We demonstrate that intraparticle effects can induce spin canting throughout a MNP via the Dzyaloshinskii-Moriya interaction (DMI). We study ~7.4 nm diameter, core/shell Fe3O4/MnxFe3−xO4 MNPs with a 0.5 nm Mn-ferrite shell. Mössbauer spectroscopy, x-ray absorption spectroscopy and x-ray magnetic circular dichroism are used to determine chemical structure of core and shell. Polarized small angle neutron scattering shows parallel and perpendicular magnetic correlations, suggesting multiparticle coherent spin canting in an applied field. Atomistic simulations reveal the underlying mechanism of the observed spin canting. These show that strong DMI can lead to magnetic frustration within the shell and cause canting of the net particle moment. These results illuminate how core/shell nanoparticle systems can be engineered for spin canting across the whole of the particle, rather than solely at the surface.

Coordination numbers and geometries form a theoretical framework for understanding and predicting materials properties. Algorithms to determine coordination numbers automatically are increasingly used for machine learning and automatic structural analysis. In this work, we introduce MaterialsCoord, a benchmark suite containing 56 experimentally-derived crystal structures (spanning elements, binaries, and ternary compounds) and their corresponding coordination environments as described in the research literature. We also describe CrystalNN, a novel algorithm for determining near neighbors. We compare CrystalNN against 7 existing near-neighbor algorithms on the MaterialsCoord benchmark, finding CrystalNN to perform similarly to several well-established algorithms. For each algorithm, we also assess computational demand and sensitivity towards small perturbations that mimic thermal motion. Finally, we 1 investigate the similarity between bonding algorithms when applied to the Materials Project database. We expect that this work will aid the development of coordination prediction algorithms as well as improve structural descriptors for machine learning and other applications.

Polarization-analyzed small-angle neutron scattering methods are used to determine the spin arrangements and experimental length scales of magnetic correlations in ordered three-dimensional assemblies of ∼ 7.4 nm diameter core-shell Fe 3 O 4 /Mn x Fe 3−x O 4 nanoparticles. In moderate to high magnetic fields, the assemblies display a canted magnetic structure where the canting direction is coherent from nanoparticle to nanoparticle, in contrast to the less extended, more single particle-like behavior for similar ferrite assemblies. The observed magnetic scattering is modeled by assuming that the interparticle dipolar coupling combined with Zeeman effects in a field leads to nanoparticle domains with preferred net spin alignments relative to packing symmetry axes. Over a range of fields and temperatures, the model qualitatively explains the observed scattering anomalies in terms of clusters that vary in area and thickness, highlighting the complex structures adopted in real, dense nanoparticle systems. The clusters often have a strong two-dimensional magnetic character which is attributed to structural stacking faults and the resulting influence of interparticle dipolar interactions for these magnetically soft nanoparticles.

Coordination numbers and geometries form a theoretical framework for understanding and predicting materials properties. Algorithms to determine coordination numbers automatically are increasingly used for machine learning and automatic structural analysis. In this work, we introduce MaterialsCoord, a benchmark suite containing 56 experimentally-derived crystal structures (spanning elements, binaries, and ternary compounds) and their corresponding coordination environments as described in the research literature. We also describe CrystalNN, a novel algorithm for determining near neighbors. We compare CrystalNN against 7 existing near-neighbor algorithms on the MaterialsCoord benchmark, finding CrystalNN to be the most accurate overall. For each algorithm, we also assess computational demand and sensitivity towards small perturbations that mimic thermal motion. Finally, we investigate the similarity between bonding algorithms when applied to the Materials Project database. We expect that this work will aid the development of coordination prediction algorithms and improve the accuracy of structural descriptors for machine learning and other applications.

Particles interacting via isotropic, multiwell pair potentials have been shown to self-assemble into a range of crystal structures, yet how the characteristics of the underlying interaction potential give rise to the resultant structure remains largely unknown. We have thus developed a functional form for the interaction potential in which all features can be tuned independently. We perform continuous parameter space searches by systematically changing pairs of parameters, controlling the various features of the interaction potential. By enforcing a repulsive first well (controlling particle interactions of the first neighbor shell), we stimulate the formation of low-coordinated assemblies. We report the self-assembly of 20 previously unknown crystal structure types, 14 of which have low coordination numbers. Despite limiting the search to a small region of the vast parameter space of possible particle interactions, a wealth of complexity and symmetry is apparent within these crystal structures, which include clathrates with empty cages and low-symmetry structures. Our findings suggest that an unknown number of previously undiscovered crystal structure configurations are possible through self-assembly, which can serve as interesting design targets for soft condensed matter synthesis.