Investigation and modification of the magnetism of epitaxial Fe structures

In this thesis, the magnetic and structural properties of layered epitaxial film systems and clusters are presented. A main achievement is the investigation of the direct correlation between magnetism and structural or morphological details of ultrathin films. For this purpose, the film structure has been accessed directly by means of surface science methods. The effect of structural changes on the magnetism were observed in-situ by magneto-optical techniques. First, epitaxial Fe films grown at low temperature (∼ 120K) on Cu(100) have been investigated. Such layers assume an fcc-crystal structure due to their interaction with the underlying Cu substrate. Within this work it is shown that the morphology of these films can be altered by annealing treatments. The thermally-induced morphological changes have direct consequences for domain wall propagation and result in increased coercivity and in modified surface anisotropy. Flat fcc-Fe layers on Cu(100) have been used as templates to form fcc-Fe/Cu/Fe trilayers with coupled perpendicular magnetization. Such systems might be of relevance for data storage applications. The perpendicular coupling is ascribed to the realignment of the magnetization of the bottom Fe layer within the stray field produced by the top Fe layer magnetization. The magnetic coupling has been investigated as a function of the thickness of the top and the bottom Fe layer as well as the Cu spacer thickness. It was found that the magneto-static interaction is a direct consequence of the fcc-structure of both Fe layers and the interface roughness. It is demonstrated that Fe films with fcc-structure and perpendicular magnetization can also be prepared on other fcc-templates, such as Pt substrates. Monatomic steps on the substrate surface are exploited to steer the growth of the film and with it the magnetism. Despite significant differences in the morphology and the atomic structure of Fe films on flat Pt(111) and stepped Pt(997), the critical thickness for the spin reorientation transition is similar on the two surfaces. However, the local atomic arrangement above three monolayer film thickness determines in-plane easy magnetization axis parallel to the step edges. For all layered systems investigated in this thesis, epitaxial strain is a the driving force which influences the film structure and triggers structural transitions. The strain dependence of the morphology and the magnetism was probed by a comparative study of Fe deposited on Pt substrates with and without a noble gas buffer layer. The formation of relaxed Fe clusters during Xe layer desorption is favored in the absence of the overlayer-substrate interaction. Striking differences in the magnetic anisotropy between the systems are attributed to magneto-elastic contributions. Measurements of the blocking temperature of the Fe clusters allow estimating the cluster size. All samples have been investigated under ultra high vacuum conditions. The study of the sample magnetic properties study was done by in-situ magneto-optical Kerr effect measurements and Kerr microscopy. Structural characterization was done by low energy electron diffraction and, in collaboration with other scientists, by scanning tunnelling microscopy.

Magnetization Reversal Dynamics in Ferromagnetic Semiconductors

Liza Herrera Diez

This thesis is dedicated to the study of the magnetization reversal dynamics in compressively strained (Ga,Mn)As and differently functionalized (Ga,Mn)As materials. In the first part the domain wall dynamics of pure (Ga,Mn)As/GaAs materials is in the focus. The changes in the magnetic anisotropy energy landscape occurring as a function of temperature are monitored in detail by different experimental techniques. These measurements provide the necessary information for the identification of the temperature ranges corresponding to different magnetic anisotropy regimes. Knowing the biaxial anisotropy and uniaxial anisotropy dominated regimes the dependence of the domain wall dynamics on the magnetic anisotropy landscape is studied. Critical changes in domain wall alignment observed by Kerr microscopy are found upon changing from biaxial to uniaxial anisotropy. These changes could be partially attributed to the tendency of the system to minimize magnetic free poles at the domain boundaries. To complement the space resolved studies of the magnetization reversal, magnetic time relaxation effects are addressed. In particular the magnetic aftereffect in (Ga,Mn)As/GaAs is studied in detail. The irreversible aftereffect is evidenced as a critical reduction of the domain wall velocity with time under a constant applied magnetic field below coercivity. This time relaxation is tracked as a function of both time and magnetic field. The measurements show that the overall relaxation is composed of two relaxation processes acting in parallel at short and long time scales. By fitting these experimental results the values of the relaxation times of both relaxation processes were obtained. By this modeling also the values of the activation volumes for two independent (Ga,Mn)As materials are estimated. In the second part of this thesis the possibilities of tuning the electrical and magnetic properties of (Ga,Mn)As by volume and surface treatments are explored. As for the volume modification, oxygen species were incorporated into the (Ga,Mn)As films by means of exposure to an oxygen plasma. The incorporation of oxygen was evidenced by depth profile X-ray photoelectron spectroscopy. This treatment is found to weaken the ferromagnetism, visible as a reduction in the Curie temperature, and to hinder the electrical transport evidenced as an increase in the electrical resistance. In agreement with theories accounting for the hole mediated ferromagnetism in (Ga,Mn)As this behaviour was related to a hole compensation mechanism arising from the presence of oxygen impurities sitting in interstitial positions of the (Ga,Mn)As Zinc blende structure. In the last part, the modulation of the electrical and magnetic properties via surface functionalization is presented. The effects produced by the adsorption of molecular species on (Ga,Mn)As are similar to those found after oxygenation, namely a strong weakening of the magnetic properties and an increase in the values of the electrical resistance. However, in this case the distinctive feature is provided by the possibility of regulating the hole quenching effect by exploiting the additional degree of freedom provided by the chemical properties of the adsorbates. The adsorbate chosen for these experiments are dye molecules that absorb light in the visible range, in this way allowing for a light modulated interaction with the substrate. Using this concept is was possible to observe a modulation of the ferromagnetic transition temperature, the coercive field and the electrical resistance upon illumination. These observations provide a proof of principle for the realization of photo-sensitized (Ga,Mn)As devices where the magnetic properties can be regulated by light.

EPFL2011

Magnetism of individual adatoms and of epitaxial monolayers

Anne Lehnert

This thesis reports on the magnetism of low coordinated Fe and Co atoms in different chemical and electronic environments. The objective of this research was to contribute to the fundamental understanding of the magnetic properties, such as magneto-crystalline anisotropy energy (MAE), orbital and spin magnetic moment, of surface supported transition metal (TM) atoms and one atomic layer thick epitaxial TM films. A detailed knowledge on the interplay of electronic hybridization and magnetic properties is mandatory to elaborate new materials with high perpendicular magnetic anisotropy and acceptable writing field for future use in magnetic recording devices. The magnetic properties of the different experimental systems were investigated by x-ray absorption spectroscopy, x-ray magnetic circular dichroism, and magneto-optical Kerr effect (MOKE) and they were correlated to the morphology obtained by scanning tunneling microscopy (STM). The first part focuses on the effect of electronic hybridization between isolated 3d TM atoms and different kinds of substrates. First, we considered 4d and 5d TM substrates known for their high magnetic polarizability due to the close onset of ferromagnetism. Deposition of single Fe and Co atoms on Rh(111), Pd(111), and Pt(111) produces an increasing MAE going from Rh to Pd and finally to Pt that we directly correlate to the increasing spin-orbit constant of the substrate interlinking the induced magnetic moment and the MAE. Further we investigated single Fe and Co atoms on two different insulating layers, namely Al2O3/Ni3Al(111) and Cu2N/Cu(001), providing an efficient decoupling of the TM 3d states from the conduction electrons of the substrates. In case of the alumina film the absorption spectra of Fe and Co show a pronounced multiplet structure. On Cu2N the multiplet features of the adatoms are less defined due to the lower thickness of the screening layer. On both insulating layers we find a common out-of-plane easy axis, highly unquenched orbital moments, and giant MAE values of several meV/atom which are due to the formation of strong anisotropic bonds with the O and N atoms, respectively. The second part is dedicated to single atom thick layers of Fe and Co deposited on Pt(111) and Rh(111). We find the MAE to be strongly enhanced compared with bulk and we establish a direct proportionality between the induced magnetic moment of the topmost substrate layer and the MAE. The study of bimetallic Fe1-xCox alloys on platinum reveal a material with high MAE (0.5 meV at the equiatomic composition), large saturation magnetization (3μB to 2μB going from Fe to Co), and perpendicular magnetization easy axis. These characteristics hint at new possibilities for the further miniaturization of the grain size in recording devices. In the last part the theoretical description of the MOKE for ultra-thin films is extended to the transverse geometry and improved analytic formulae for the polar and longitudinal geometry are presented. This finding was used to optimize the Kerr signal for a new MOKE setup which is fully integrated in an ultrahigh vacuum chamber combining in situ MOKE and STM. The setup performance was demonstrated for a continuous film of 0.9 monolayers (ML) Co/Rh(111) with in-plane easy axis and for a superlattice of nanometric double layer Co islands on Au(11,12,12) with out-of-plane easy axis. The detection limit is 0.5 ML for transverse and 0.1 ML for polar Kerr geometry corresponding for island superlattices with the density of Co/Au(11,12,12) to islands composed of about 50 atoms. Moreover, the setup holds two independent ways to measure the MAE which is either by thermally induced magnetization reversal or by applying a torque onto the magnetization by turning the magnetic field. Both ways yield similar results for 1.1 ML Co/Au(11,12,12).

EPFL2009

Structure and magnetism of atomically thin Fe layers on flat and vicinal Pt surfaces

Harald Brune, Pietro Gambardella, Klaus Kern, Stefano Rusponi, Violetta Sessi

Ultrathin Fe films on Pt substrates have been investigated under ultrahigh vacuum conditions by scanning tunneling microscopy, low energy electron diffraction, magneto-optical Kerr effect, x-ray magnetic circular dichroism measurements, and Kerr microscopy. We present a comparison between Fe films on flat Pt(111) and stepped Pt(997), with particular focus on the magnetic anisotropy in the submonolayer thickness range below 0.2 monolayer coverage, and above the spin reorientation transition at 3 monolayer thickness. The comparison of structure and magnetism suggests that the perpendicular easy axis found for films thinner than three monolayers is due to dominating contributions from both film interfaces to the anisotropy energy. The Fe-Pt interface contribution has its origin in the hybridization of the Fe 3d with the Pt 5d band. The in-plane magnetic anisotropy above 3 atomic layers film thickness can be correlated directly with peculiarities of the film structure.