Combinatorial evaluation of phase formation and magnetic properties of FeMnCoCrAl high entropy alloy thin film library.

We report on the influence of the Al content (from 3.5 to 54 at.%) on phase formation and magnetic properties in FeMnCoCrAl high entropy alloy thin film libraries. Al additions to FeMnCoCr crystallizing in the alpha-Mn structure cause the formation of the body centered cubic (BCC) structure. This is consistent with density functional theory predictions as Al additions give rise to a larger stability for the BCC phase compared to the face centered cubic phase (FCC) which can be rationalized by the formation of a pseudogap at the Fermi level indicating the stabilization of the BCC phase over the FCC phase. Al additions to paramagnetic FeMnCoCr induce ferromagnetism. The largest saturation magnetization was measured for the film containing 8 at.% of Al. As the concentration of non-ferromagnetic Al is increased beyond 8 at.%, the number density of the ferromagnetic species is decreased causing a concomitant decrease in magnetization. This trend is consistent with ab initio predictions of the Al concentration induced changes in the magnetic moment. Based on the experimental and theoretical results presented here the effect of the Al concentration on the phase formation and the magnetic properties of FeMnCoCrAl thin film library can be rationalized.

Strain and electric-field control of magnetism in supercrystalline iron oxide nanoparticle-BaTiO3 composites.

The manipulation of the magnetism of self-assembled iron oxide nanoparticle (NP) monolayers on top of BaTiO3 (BTO) single crystals is reported. We observe strain induced magnetoelectric coupling (MEC) as shown by measurements of both the magnetization and magneto-electric AC susceptibility (MEACS). The magnetization, coercivity, remanent magnetization and MEACS signal as a function of temperature show abrupt jumps at the BTO phase transition temperatures. Hereby the jump values are opposite for in-plane and out-of-plane measurements. Grazing incidence small angle X-ray scattering (GISAXS) and scanning electron microscopy (SEM) confirm a hexagonal close-packed supercrystalline order of the NP monolayers. Cross-sectional scanning transmission electron microscopy (STEM) experiments provide information about the layer structure of the sample. This work opens up viable possibilities for fabricating energy-efficient electronic devices by self-assembly techniques.

Polarized neutron reflectivity from monolayers of self-assembled magnetic nanoparticles.

We prepared monolayers of iron oxide nanoparticles via self-assembly on a bare silicon wafer and on a vanadium film sputter deposited onto a plane sapphire substrate. The magnetic configuration of nanoparticles in such a dense assembly was investigated by polarized neutron reflectivity. A theoretical model fit shows that the magnetic moments of nanoparticles form quasi domain-like configurations at remanence. This is attributed to the dipolar coupling amongst the nanoparticles.

Growth modes of nanoparticle superlattice thin films.

We report on the fabrication and characterization of iron oxide nanoparticle thin film superlattices. The formation into different film morphologies is controlled by tuning the particle plus solvent-to-substrate interaction. It turns out that the wetting vs dewetting properties of the solvent before the self-assembly process during solvent evaporation plays a major role in determining the resulting film morphology. In addition to layerwise growth three-dimensional mesocrystalline growth is also evidenced. The understanding of the mechanisms ruling nanoparticle self-assembly represents an important step towards the fabrication of novel materials with tailored optical, magnetic or electrical transport properties.

Self-assembled iron oxide nanoparticle multilayer: x-ray and polarized neutron reflectivity.

We have investigated the structure and magnetism of self-assembled, 20 nm diameter iron oxide nanoparticles covered by an oleic acid shell for scrutinizing their structural and magnetic correlations. The nanoparticles were spin-coated on an Si substrate as a single monolayer and as a stack of 5 ML forming a multilayer. X-ray scattering (reflectivity and grazing incidence small-angle scattering) confirms high in-plane hexagonal correlation and a good layering property of the nanoparticles. Using polarized neutron reflectivity we have also determined the long range magnetic correlations parallel and perpendicular to the layers in addition to the structural ones. In a field of 5 kOe we determine a magnetization value of about 80% of the saturation value. At remanence the global magnetization is close to zero. However, polarized neutron reflectivity reveals the existence of regions in which magnetic moments of nanoparticles are well aligned, while losing order over longer distances. These findings confirm that in the nanoparticle assembly the magnetic dipole-dipole interaction is rather strong, dominating the collective magnetic properties at room temperature.

Template-assisted self-assembly of individual and clusters of magnetic nanoparticles.

The deliberate control over the spatial arrangement of nanostructures is the desired goal for many applications such as, for example, in data storage, plasmonics or sensor arrays. Here we present a novel method to assist the self-assembly process of magnetic nanoparticles. The method makes use of nanostructured aluminum templates obtained after anodization of aluminum discs and the subsequent growth and removal of the newly formed alumina layer, resulting in a regular honeycomb-type array of hexagonally shaped valleys. The iron oxide nanoparticles, 20 nm in diameter, are spin-coated onto the surface of honeycomb nanostructured Al templates. Depending on the size, each hexagon site can host up to 30 nanoparticles. These nanoparticles form clusters of different arrangements within the valleys, such as collars, chains and hexagonally closed islands. Ultimately, it is possible to isolate individual nanoparticles. The strengths of the magnetic interaction between particles in a cluster are probed using the memory effect known from the coupled state in superspin glass systems.

Structural and magnetic characterization of self-assembled iron oxide nanoparticle arrays.

We report about a combined structural and magnetometric characterization of self-assembled magnetic nanoparticle arrays. Monodisperse iron oxide nanoparticles with a diameter of 20 nm were synthesized by thermal decomposition. The nanoparticle suspension was spin-coated on Si substrates to achieve self-organized arrays of particles and subsequently annealed at various conditions. The samples were characterized by x-ray diffraction, and bright and dark field high resolution transmission electron microscopy. The structural analysis is compared to magnetization measurements obtained by superconducting quantum interference device magnetometry. We can identify either multi-phase Fe(x)O/γ-Fe(2)O(3) or multi-phase Fe(x)O/Fe(3)O(4) nanoparticles. The Fe(x)O/γ-Fe(2)O(3) system shows a pronounced exchange bias effect which explains the peculiar magnetization data found for this system.

Evidence for core-shell magnetic behavior in antiferromagnetic Co3O4 nanowires.

Employing magnetometry measurements, we have studied Co3O4 nanowires focusing on the core-shell behavior. We find two magnetic contributions, i.e., a regular antiferromagnetic and an additional irreversible one. The first contribution can be attributed to the antiferromagnetically ordered wire cores. The nature of the second one can be identified using thermoremanent and isothermoremanent magnetizaton curves as magnetic fingerprints of the irreversible magnetization. We conclude that the nanowire shell behaves like a two-dimensional diluted antiferromagnet in a field.

Modes of periodic domain wall motion in ultrathin ferromagnetic layers.

Magnetization reversal in a periodic magnetic field is studied on an ultrathin, ultrasoft ferromagnetic Pt/Co(0.5 nm)/Pt trilayer exhibiting weak random domain wall (DW) pinning. The DW motion is imaged by polar magneto-optic Kerr effect microscopy and monitored by superconducting quantum interference device susceptometry. In close agreement with model predictions, the complex linear ac susceptibility corroborates the dynamic DW modes segmental relaxation, creep, slide, and switching.

Depth profile of uncompensated spins in an exchange bias system.

We have used the unique spatial sensitivity of polarized neutron and soft x-ray beams in reflection geometry to measure the depth dependence of magnetization across the interface between a ferromagnet and an antiferromagnet. The net uncompensated magnetization near the interface responds to applied field, while uncompensated spins in the antiferromagnet bulk are pinned, thus providing a means to establish exchange bias.

Domain wall relaxation, creep, sliding, and switching in superferromagnetic discontinuous Co(80)Fe(20)/Al(2)O3 multilayers.

The ac susceptibility of a superferromagnetic discontinuous multilayer [Co(80)Fe20(1.4 nm)/Al(2)O3(3 nm)](10) is measured as a function of temperature, frequency, and field amplitude and compared to static and dynamic hysteresis loops. Its properties are successfully mapped onto the predicted [T. Nattermann, V. Pokrovsky, and V. M. Vinokur, Phys. Rev. Lett. 87, 197005 (2001)]] dynamical phase transitions, which link the relaxation, creep, sliding, and switching regimes of pinned domain walls.