Magnetic states in low-pinning high-anisotropy material nanostructures suitable for dynamic imaging

We present magnetic domain states in a material configuration with high (perpendicular) magnetic anisotropy and particularly low magnetic pinning. This material, a B-doped Co/Pt multilayer configuration, exhibits a strong magnetic contrast in x-ray transmission experiments, making it apt for dynamic imaging with modern synchrotron techniques, providing high spatial and high temporal resolution simultaneously. By analyzing the static spin structures in nanodisks at variable external fields, we show that CoB/Pt multilayers exhibit low enough domain wall pinning to manipulate the domain pattern with weak stimuli and in particular to move domains and domain walls. We demonstrate in a proof-of-principle experiment using pump-probe x-ray holographic imaging that moderate magnetic fields can induce elastic and deterministic and hence repeatable small variations of the domain configuration in CoB/Pt multilayers, which is the key to perform high-resolution imaging of the domain wall motion to gain insight to the details of the local magnetization dynamics. DOI: 10.1103/PhysRevB.87.134422

Nanoscale superparamagnetic composite particles for biomedical applications

Mathieu Chastellain

The present thesis report deals about the material scientists contribution to the interdisciplinary European project "MAGNANOMED" involving people having very different backgrounds (physicist, chemists, biochemists, veterinary surgeons, ...). The work carried out was aimed at the development of iron oxide based nanoscale superparamagnetic composite particles for biomedical applications. Particles showing a superparamagnetic behaviour are of particular interest as they are sensitive to magnetic fields without retaining magnetisation after removal of the latter. Not only superparamagnetic particles can be guided, but they also exhibit heating properties when submitted to appropriate alternating magnetic fields. These characteristics make them promising for targeted applications where they could act as careers as well as activators. The local temperature increase can be used for confined control release of linked entities or to modify specific cells activities in a well defined area. Moreover iron oxide nanoparticles can be used for magnetic resonance imaging enhancement. No single sample could meet the requirements imposed by every application mentioned above, so the chosen strategy was first to synthesize and thoroughly characterize iron oxide nanoparticles. In a second step, the particles would serve as primary building blocks for higher order composite structures or "beads" (with one or more iron oxide cores) to be formed according to the specific needs of every particular application. The surface tailoring, so that to ensure the desired properties in physiological media and allow further functionalisation, consisted in an important part of the work. Despite the many works carried out in the field over the past decades, the needs for well controlled biocompatible superparamagnetic beads are not only important but also growing. A focus was made on three specific applications: hyperthermia (controlled heating in a well defined body area by means of an external alternating magnetic field), drug delivery (magnetic targeted drug release) and DNA purification (magnetically driven separation in vitro). A supplementary application called ferrofluid actuated micro pump is also described as it turned out that a synthesis side product could be judiciously used in this field. The achievements realized allowed to define a reproducible and versatile synthesis route, which fulfils the above mentioned criteria as summarised in the following. Iron oxide particles, which physical properties could be well controlled, were shown to generate heat when submitted to an external magnetic field suitable for medical applications. The measured power dissipated could be successfully related to the particles and field characteristics using a theoretical approach and the tremendous influence of particles size distribution was highlighted. Polyvinyl alcohol coated iron oxide particles were produced for drug delivery. Biocompatibility was asserted based on both in vitro and in vivo experiments. The particles bio-distribution could be influenced by means of a constant magnetic field (magnet) and depending on the coating nature (presence of functional groups), the cellular uptake could be controlled. Silica beads with a homogeneous iron oxide particles space distribution were synthesised in view of DNA separation using a novel approach. The bead size could be adjusted in the 20 nanometres up to several microns range. Preliminary classical plasmid automated purification experiments revealed a competitive separation yield. These results are promising in view of the final targeted application in currently developed quicker automated processes. A highly concentrated iron oxide suspension (ferrofluid) showing suitable colloidal stability was successfully applied in micropumps actuated by means of a magnetically induced ferrofluid motion. The obtained pumping characteristics such as backpressure and flow rate were better then described in literature for similar devices using water based ferrofluids. AFM 3D-view of iron oxide particles coated with polyvinyl alcohol, average height 9 nm (left) and Stonehenge monument in Britain, heaviest stone 50 tons (right). "In its day, the construction of Stonehenge was an impressive engineering feat, requiring commitment, time and vast amounts of manual labour" [http://www.britannia.com/ history/h7.html] (see appendix 12.6). Nowadays, this remark still holds for Nano-stonehenge synthesis ...

EPFL2004

Magnetism of Single Adatoms and Small Adsorbed Clusters Investigated by Means of Low-Temperature STM

Quentin Dubout

This thesis works reports on the magnetic properties of single transition metal atoms and hydrogenated compounds adsorbed on crystal surfaces. It is an experimental study, based on scanning tunneling microscopy (STM), initiated by the project of demonstrating the existence of magnetic remanence for single adsorbed atoms (adatoms). All the measurements have been performed with a scanning tunneling microscope operating at 0.4 K and equipped with 8.5 T superconducting coils. The investigated systems are cobalt atoms, pure and hydrogenated (cobalt hydrides), adsorbed on Pt(111) and graphene on Pt(111) surfaces. In the first case, we have immediately been confronted to the presence of cobalt hydrides on the surface. Three types of hydrides (CoH, CoH2, and CoH3) have been identified, quite different from the clean adatoms, and readily distinguished by their tunnel spectrum (STS). Twoofthesehydridesdisplaylow-energyvibrationalmodes(1−30meV),identifiedbytheir absence of response to a magnetic field, the effect of an isotopic substitution, and by comparison with known systems. The three hydrides can be deprotonated applying a sufficient voltage between tip and sample. CoH2 on Pt(111) presents a Kondo resonance, due to a half-integer spin (S = 3/2) and a peculiar magnetic anisotropy. This system corresponds to the first demonstration of the appearance of the Kondo effect upon hydrogen adsorption. The results of several attempts to observe remanence for single cobalt adatoms on Pt(111) with spin-polarized scanning tunneling microscopy (SP-STM) are also presented and discussed. The second system differs from the first one in the presence of a graphene layer on the Pt surface. The first experimental determination of the magnetic moment and magnetic anisotropy of adatoms on graphene is reported in this thesis. A magnetic moment of (2.2 ± 0.4) μB was measured by spin-excitation spectroscopy (SES), as well as a hard magnetization axis with an anisotropy energy of 8.1 ± 0.4 meV. This value, comparable to the record value of single cobalt atoms on Pt(111), has been mainly attributed to the strong hybridization between cobalt and graphene. Ab initio calculations confirmed our observations. Graphene thus represents an extremely promising substrate for future applications in nanoscale magnetism and spintronics. This system also exhibits three different cobalt hydrides in addition to the clean atoms. Their respective chemical composition, CoH, CoH2, and CoH3, was determined by direct comparison between high resolution STM images and simulated images obtained from ab initio calculated atomic structures. A controlled deprotonation method is presented. CoH3 is the only hydride to display spin excitations. Its magnetic moment is comparable to that of clean cobalt, it presents a hard magnetization axis as well, however, its magnetic anisotropy energy is sensibly lower, 1.7 ± 0.05 meV. The other two hydrides display vibrational excitations only. The effect of hydrogen on the magnetic properties of metal adatoms is therefore very strong in this system as well, and must be taken into account in future studies, hydrogen being a very common contaminant in ultra-high vacuum set-ups. Finally, a detailed study of the structure graphene mono- and bilayers on Ru(0001) was realized. Two different stackings, AB and AA, have been identified for the bilayers, the last one not observed to date for this system. The moiré structure of monolayer graphene and of this last type of bilayer has been determined: (11.57×11.57)R4.3◦ and (10.54×10.54)R4.7◦, respectively. Moreover, C-C bond distortions of more than 10%, observed in the STM images, have been studied in detail. A quantitative comparison with ab initio calculations allowed to identify their origin as the tilt of the graphene π-orbitals. These distortions are therefore purely artificial. This is an important result for future scanning tunneling microscopy studies of graphene.

EPFL2013

Field-dependent roughness of moving domain walls in a Pt/Co/Pt magnetic thin film

Elisabeth Agoritsas

The creep motion of domain walls driven by external fields in magnetic thin films is described by universal features related to the underlying depinning transition. One key parameter in this description is the roughness exponent characterizing the growth of fluctuations of the domain wall position with its longitudinal length scale. The roughness amplitude, which gives information about the scale of fluctuations, however, has received less attention. Albeit their relevance, experimental reports of the roughness parameters, both exponent and amplitude, are scarce. We report here experimental values of the roughness parameters for different magnetic field intensities in the creep regime at room temperature for a Pt/Co/Pt thin film. The mean value of the roughness exponent is ζ=0.74, and we show that it can be rationalized as an effective value in terms of the known universal values corresponding to the depinning and thermal cases. In addition, it is shown that the roughness amplitude presents a significant increase with decreasing field. These results contribute to the description of domain wall motion in disordered magnetic thin systems.