Ultrafast Demagnetization Control in Magnetophotonic Surface Crystals.

Magnetic memory combining plasmonics and magnetism is poised to dramatically increase the bit density and energy efficiency of light-assisted ultrafast magnetic storage, thanks to nanoplasmon-driven enhancement and confinement of light. Here we devise a new path for that, simultaneously enabling light-driven bit downscaling, reduction of the required energy for magnetic memory writing, and a subtle control over the degree of demagnetization in a magnetophotonic surface crystal. It features a regular array of truncated-nanocone-shaped Au-TbCo antennas showing both localized plasmon and surface lattice resonance modes. The ultrafast magnetization dynamics of the nanoantennas show a 3-fold resonant enhancement of the demagnetization efficiency. The degree of demagnetization is further tuned by activating surface lattice modes. This reveals a platform where ultrafast demagnetization is localized at the nanoscale and its extent can be controlled at will, rendering it multistate and potentially opening up so-far-unforeseen nanomagnetic neuromorphic-like systems operating at femtosecond time scales controlled by light.

Self-assembly and percolation in two dimensional binary magnetic colloids.

We study the self-assembly of branching-chain networks and crystals in a binary colloidal system with tunable interactions. The particle positions are extracted from microscopy images and order parameters are extracted by image processing and statistical analysis. With these, we construct phase diagrams with respect to particle density, ratio and interaction. In order to draw a more complete picture, we complement the experiments with computer simulations. We establish a region in the phase diagram, where bead ratios and interactions are symmetric, promoting percolated structures.

Statistical analysis of phase formation in 2D colloidal systems.

Colloidal systems offer unique opportunities for the study of phase formation and structure since their characteristic length scales are accessible to visible light. As a model system the two-dimensional assembly of colloidal magnetic and non-magnetic particles dispersed in a ferrofluid (FF) matrix is studied by transmission optical microscopy. We present a method to statistically evaluate images with thousands of particles and map phases by extraction of local variables. Different lattice structures and long-range connected branching chains are observed, when tuning the effective magnetic interaction and varying particle ratios.

Light Localization and Magneto-Optic Enhancement in Ni Antidot Arrays.

We reveal an explicit strategy to design the magneto-optic response of a magneto-plasmonic crystal by correlating near- and far-fields effects. We use photoemission electron microscopy to map the spatial distribution of the electric near-field on a nanopatterned magnetic surface that supports plasmon polaritons. By using different photon energies and polarization states of the incident light we reveal that the electric near-field is either concentrated in spots forming a hexagonal lattice with the same symmetry as the Ni nanopattern or in stripes oriented along the Γ-K direction of the lattice and perpendicular to the polarization direction. We show that the polarization-dependent near-field enhancement on the patterned surface is directly correlated to both the excitation of surface plasmon polaritons on the patterned surface as well as the enhancement of the polar magneto-optical Kerr effect. We obtain a relationship between the size of the enhanced magneto-optical behavior and the polarization and wavelength of optical excitation. The engineering of the magneto-optic response based on the plasmon-induced modification of the optical properties introduces the concept of a magneto-plasmonic meta-structure.

Surface plasmons and magneto-optic activity in hexagonal Ni anti-dot arrays.

The influence of surface plasmons on the magneto-optic activity in a two-dimensional hexagonal array is addressed. The experiments were performed using hexagonal array of circular holes in a ferromagnetic Ni film. Well pronounced troughs are observed in the optical reflectivity, resulting from the presence of surface plasmons. The surface plasmons are found to strongly enhance the magneto-optic response (Kerr rotation), as compared to a continuous film of the same composition. The influence of the hexagonal symmetry of the pattern on the coupling between the plasmonic excitations is demonstrated, using optical diffraction measurements and theoretical calculations of the magneto-optic and of the angular dependence of the optical activity.

Ultrafast demagnetization in a ferrimagnet under electromagnetic field funneling.

The quest to improve the density, speed and energy efficiency of magnetic memory storage has led to the exploration of new ways of optically manipulating magnetism at the ultrafast time scale, in particular in ferrimagnetic alloys. While all-optical magnetization switching is well-established on the femtosecond timescale, lateral nanoscale confinement and thus the potential significant reduction of the size of the magnetic element remains an outstanding challenge. Here we employ resonant electromagnetic energy funneling through plasmon nanoantennas to influence the demagnetization dynamics of a ferrimagnetic TbCo alloy thin film. We demonstrate how Ag nanoring-shaped antennas under resonant optical femtosecond pumping reduce the overall demagnetization in the underlying films up to three times compared to non-resonant illumination. We attribute such a substantial reduction to the nanoscale confinement of the demagnetization process. This is qualitatively supported by the electromagnetic simulations that strongly evidence the resonant optical energy-funneling to the nanoscale from the nanoantennas into the ferrimagnetic film. This observation is an important step for reaching deterministic ultrafast all-optical magnetization switching at the nanoscale in such systems, opening a route to develop nanoscale ultrafast magneto-optics.

Structure and magnetic properties of hcp and fcc nanocrystalline thin Ni films and nanoparticles produced by radio frequency magnetron sputtering.

We report on the growth of thin Ni films by radio frequency magnetron sputtering in Ar-plasma. The growth temperature was about 350 K and the films were deposited on various substrates such as glass, silicon, sapphire and alumina. The thickness of the thinnest films was estimated by the appearance of Kiessig fringes up to about 2theta = 8 degrees in the small-angle X-ray diffraction pattern, as expected for high-quality atomically-flat thin films. With the help of this, a quartz balance system was calibrated and used for measuring the thickness of thicker samples with an accuracy of better than 5%. Structural characterization via X-ray diffraction and high resolution transmission electron microscopy revealed an Ar-gas pressure window, where single phase hcp Ni films may be grown. The magnetic response of the Ni films was checked at room temperature via a newly established and fully automatic polar magneto-optic Kerr effect magnetometer. The hcp films show no magnetic response. Interestingly, the magnetic saturation field of fcc films deposited at low Ar pressure is comparable to the one of bulk Ni, while the one of fcc films deposited at high Ar pressures is decreased, revealing the presence of residual strain in the films. Finally, it is shown that it is possible to form films which contain magnetic Ni fcc nanoparticles in a non-magnetic hcp matrix, i.e., a system interesting for technological applications demanding a single Ni target for its production.

Magnetic force microscopy on nanocrystalline Co films.

Pioneer works in ultrathin magnetic films have shown perpendicular magnetic domains in the demagnetized state. The source of this perpendicular anisotropy is the interface anisotropy developed at the interface. Similar domains could be observed in tetragonally distorted ultrathin films due to the magnetoelastic anisotropy. On the other hand, single-crystalline hexagonal close packed (hcp) Co films when grown epitaxially with the c-axis oriented perpendicular to the film plane may show perpendicular stripe magnetic domains even up to a thickness of about 500 nm. In that case the source of perpendicular anisotropy was the magnetocrystalline anisotropy of bulk Co, which favors the c-axis. In this work, we have grown by radio frequency magnetron sputtering Co films in the thickness range 15-4500 nm. We have used various substrates, such as Corning glass, silicon and Al-foil. The substrate temperature was about 350 K. The films have been found by X-ray diffraction experiments to present various structures and textures depending on the preparation conditions, mainly the Ar-pressure and deposition rate. Stripe- and labyrinth-like domain configurations are observed in films textured along the c-axis, and in films with a mixture of hcp and fcc grains, repectively. Films which show mainly fcc or amorphous structure do not form perpendicular domains. The results are discussed with respect to magnetization loops.

A simple cost-effective sputtering-based method for micropatterning and materials microstructuring.

Patterning of semiconductors results in the fabrication of micro- and nano-structures, which are desired in modern technologies. Such a patterning is usually realized with the help of e-beam-, high-energy ion-, X-ray- or laser-assisted techniques, which demand expensive equipments. In this work we present a simple cost-effective method realized via a radio-frequency driven magnetron-sputtering head in high vacuum. The target is a silicon wafer masked with metallic grids. If the grid is magnetic, e.g., nickel, it is attracted by the magnetic forces of the magnetron, otherwise, magnetic clamps are used. Soft sputtering conditions, i.e., 30-100 Watts are used and the result is a well-ordered micropatterning of the surface with nicely formed pits the size of which is entirely determined by the grid size and the depth by the sputtering power and time. The pits are monitored with the help of Optical and Atomic Force Microscopy. If the masked micropatterned silicon wafer is then used as a substrate, the pits may be partially filled by a material. As a first example we present square-like Co microstructures. The magnetic signal of these Co microstructures is recorded with the help of a computer-driven magneto-optic Kerr effect home-made magnetometer. This patterned material may be used in magnetic recording technology. More examples include the formation of Cu-microcolumns and Pt film microframeworks. For the latter ones, an etching process is applied to prepare porous silicon networks with photoluminescence, which may be used in optoelectronics.

Nanolithographic templates using diblock copolymer films on chemically heterogeneous substrates.

The orientation of the lamellae formed by the phase separation of symmetric diblock copolymer thin films is strongly affected by the wetting properties of the polymer blocks with respect to the substrate. On bare silicon wafers the lamellae of polystyrene-b-polymethylmethacrylate thin films tend to order parallel to the wafer surface, with the polymethylmethacrylate block preferentially wetting silicon. We have developed a methodology for inducing the arrangement of lamellae perpendicular to the substrate by using chemically modified substrates. This is done by chemisorbing a self-assembled monolayer of thiol-terminated alkane chains on thin gold films deposited on silicon wafers. We also show that it is possible to spatially control the perpendicular orientation of the lamellae at sub-micron length scales by using simple chemical patterns and etch them, in order to produce nanolithographic templates. This method may be of great technological interest for the preparation of well-defined templates using block copolymer thin films.

The impact of nanoscale compositional variation on the properties of amorphous alloys.

The atomic distribution in amorphous FeZr alloys is found to be close to random, nevertheless, the composition can not be viewed as being homogenous at the nm-scale. The spatial variation of the local composition is identified as the root of the unusual magnetic properties in amorphous [Formula: see text] alloys. The findings are discussed and generalised with respect to the physical properties of amorphous and crystalline materials.

Ising-like behaviour of mesoscopic magnetic chains.

We demonstrate an experimental realization of the short range magnetic order in a one-dimensional Ising chain using fabricated mesospins. We confirm an excellent agreement between the experimental findings and simulations obtained using the original Ising model. In particular, we are able to show that the thermal behaviour of the mesoscopic Ising chain dominates over the thermal behaviour of the individual mesospins themselves, confirming that fabricated mesospins can be viewed as artificial magnetic atoms.

Large uniaxial magnetostriction with sign inversion at the first order phase transition in the nanolaminated Mn2GaC MAX phase.

In 2013, a new class of inherently nanolaminated magnetic materials, the so called magnetic MAX phases, was discovered. Following predictive material stability calculations, the hexagonal Mn2GaC compound was synthesized as hetero-epitaxial films containing Mn as the exclusive M-element. Recent theoretical and experimental studies suggested a high magnetic ordering temperature and non-collinear antiferromagnetic (AFM) spin states as a result of competitive ferromagnetic and antiferromagnetic exchange interactions. In order to assess the potential for practical applications of Mn2GaC, we have studied the temperature-dependent magnetization, and the magnetoresistive, magnetostrictive as well as magnetocaloric properties of the compound. The material exhibits two magnetic phase transitions. The Néel temperature is T N ~ 507 K, at which the system changes from a collinear AFM state to the paramagnetic state. At T t = 214 K the material undergoes a first order magnetic phase transition from AFM at higher temperature to a non-collinear AFM spin structure. Both states show large uniaxial c-axis magnetostriction of 450 ppm. Remarkably, the magnetostriction changes sign, being compressive (negative) above T t and tensile (positive) below the T t . The sign change of the magnetostriction is accompanied by a sign change in the magnetoresistance indicating a coupling among the spin, lattice and electrical transport properties.

Grazing-incidence small-angle neutron scattering from structures below an interface.

Changes of scattering are observed as the grazing angle of incidence of an incoming beam increases and probes different depths in samples. A model has been developed to describe the observed intensity in grazing-incidence small-angle neutron scattering (GISANS) experiments. This includes the significant effects of instrument resolution, the sample transmission, which depends on both absorption and scattering, and the sample structure. The calculations are tested with self-organized structures of two colloidal samples with different size particles that were measured on two different instruments. The model allows calculations for various instruments with defined resolution and can be used to design future improved experiments. The possibilities and limits of GISANS for different studies are discussed using the model calculations.

Effective band gap of Si nanocrystals embedded in SiO2 matrix.

Using a formulation of the Hartree-Fock formalism with the potential morphing method in the effective mass approximation, we calculate the effective band gap of Si nanocrystals embedded in SiO2 matrix without the existence of polysilane, as a function of their diameter in the size range 1-3.5 nm. Our results are in better agreement with the experimental data, in comparison with other existing theoretical data. For diameter smaller than 2 nm our results have the same tendency with the existing theoretical results, e.g., the discrepancy between theory and experiment seems to be essential.

Non-magnetic hexagonal nanocrystalline ni films grown by radio frequency magnetron sputtering.

Nanoscale Ni films in the thickness range 15-500 nm were grown on various substrates, such as amorphous glass, single crystalline silicon and sapphire, and polycrystalline alumina, at a temperature of about 350 K by radio frequency magnetron sputtering. It is demonstrated, via X-ray diffraction and high-resolution transmission electron microscopy, that there is an Ar-gas pressure window that favors the growth of stable single-phase hexagonal nanocrystalline Ni films regardless of the film thickness and the kind of the substrate. At lower or higher Ar pressures the films grow in the regular face centered cubic phase of Ni. The structural habits are attributed to differences in the kinetic energy of the Ni atoms impinging on the substrates. Superconducting quantum interference device magnetometry measurements reveal that the hexagonal films show zero magnetic response down to liquid Helium temperature. This result is discussed with respect to earlier first principle calculations and to experimental results on Ni nanoparticles.

Phase formation in colloidal systems with tunable interaction.

Self-assembly is one of the most fascinating phenomena in nature and is one key component in the formation of hierarchical structures. The formation of structures depends critically on the interaction between the different constituents, and therefore the link between these interactions and the resulting structure is fundamental for the understanding of materials. We have realized a two-dimensional system of colloidal particles with tunable magnetic dipole forces. The phase formation is studied by transmission optical microscopy and a phase diagram is constructed. We report a phase transition from hexagonal to random and square arrangements when the magnetic interaction between the individual particles is tuned from antiferromagnetic to ferrimagnetic.

Thermal fluctuations in artificial spin ice.

Artificial spin ice systems have been proposed as a playground for the study of monopole-like magnetic excitations, similar to those observed in pyrochlore spin ice materials. Currents of magnetic monopole excitations have been observed, demonstrating the possibility for the realization of magnetic-charge-based circuitry. Artificial spin ice systems that support thermal fluctuations can serve as an ideal setting for observing dynamical effects such as monopole propagation and as a potential medium for magnetricity investigations. Here, we report on the transition from a frozen to a dynamic state in artificial spin ice with a square lattice. Magnetic imaging is used to determine the magnetic state of the islands in thermal equilibrium. The temperature-induced onset of magnetic fluctuations and excitation populations are shown to depend on the lattice spacing and related interaction strength between islands. The excitations are described by Boltzmann distributions with their factors in the frozen state relating to the blocking temperatures of the array. Our results provide insight into the design of thermal artificial spin ice arrays where the magnetic charge density and response to external fields can be studied in thermal equilibrium.

Dimensionality and confinement effects in δ-doped Pd(Fe) layers.

We address the dimensionality aspects of the magnetic ordering in δ-doped Pd(Fe) structures. The key property we investigate, via magneto-optic Kerr measurements, is the magnetization induced by iron in palladium, over a wide temperature range 5 K < T < 300 K. The dimensional crossover we observe cannot be rationalized on the basis of structural considerations alone, since we find the dimensionality of the low temperature and of the critical region can differ. We discuss the crossover in terms of the temperature dependence of the magnon modes, giving rise to lower dimensionality at low temperatures.