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Structure and magnetocrystalline anisotropy of interlayer modified ultrathin epitaxial magnetite films on MgO(001)

In this thesis the influence of different growth conditions on the structural and the magnetic
properties of magnetite were analyzed. Therefore, ultrathin Fe3O4 films were grown on
MgO(001) substrates, on NiO, and on Fe pre-covered MgO(001) substrates.
In the first part of this thesis magnetite films with different film thicknesses were deposited
directly on MgO by RMBE to investigate the thickness dependence of the anomalous strain
and the in-plane magnetic anisotropy. Surface sensitive methods like XPS and LEED have
shown that all films in the investigated thickness range are stoichiometric and epitactic magnetite.
Bulk sensitive XRD experiments at the specular rod point to well-ordered films with
homogenous film thickness indicated by the distinct Laue oscillations. However, the vertical
layer distances are smaller than expected even for strained magnetite. Raman measurements
were carried out to clarify this contradiction between surface sensitive and bulk sensitive
measurements. While the 20 nm and 30 nm films exhibit the typical bands for magnetite,
no distinct bands can be observed for the 7.6 nm film. Due to this results we first assume
a partial formation of a thin maghemite layer on top of the uncapped magnetite film under
ambient conditions. Nevertheless, additional XPS measurement exclude the complete oxidation
of magnetite to maghemite since there is no significantly increased Fe3+-signal visible.
Thus, the low vertical layer distance can be attributed to the presence of APBs causing an
anomalous strain relaxation as reported in literature. Although all films feature ferromagnetic
behavior there are differences in the characteristic of the magnetic in-plane anisotropy.
The 7.6 nm film has an in-plane magnetic isotropy while the 20 nm and 30 nm film have an
in-plane fourfold magnetic anisotropy. Here, the fourfold magnetic anisotropy is stronger for
the 20 nm magnetite film than for the 30 nm film. The critical film thickness for the transition
from magnetic isotropy to magnetic fourfold anisotropy may be influenced by film thickness
and lattice strain induced by the substrate.
The second part of this thesis features the thickness dependence of the structural quality of
Fe3O4/NiO bilayers. Each film of the Fe3O4/NiO bilayer on MgO(001) have been successfully
grown by RMBE. LEED and XPS experiments have proven that the surface near regions of
the distinct films have high structural and stoichiometric properties.
Here, too, the detailed ’bulk’ structural characterization of Fe3O4/NiO bilayers were carried
out using XRD. It was shown that the Fe3O4 films grow homogeneously and smoothly on NiO
films if the NiO film thickness is below 24 nm. Above this NiO film thickness the structural
quality of the magnetite films gets distinctly worse. This behavior can be attributed to the
fact that the interface roughness between NiO and Fe3O4 depends on the NiO film thickness.
The roughness of the 3 nm NiO film is rather small and it is rising obviously with increasing
NiO film thickness. Thus, the structural quality of the magnetite films grown on 30 nm NiO
films is constantly reduced with increasing magnetite film thickness since the quality of the
Fe3O4 films is influenced by the quality of the Fe3O4/NiO interface.
In the third study the influence of initial iron buffer layers on the magnetic properties of magnetite
grown on MgO(001) substrates has been investigated. In situ XPS and LEED indicate that the structural and stoichiometric properties of the surface near region of the magnetite
films are not influenced by the iron buffer layer. However, the structural and magnetic properties
of the whole film have changed compared to magnetite grown directly on MgO as shown
by XRD and MOKE. The crystalline quality is poor and the magnetic easy axis of the magnetic
in-plane anisotropy is rotated by 45◦ compared to magnetite films grown directly on
MgO. Both crystalline quality and the rotation of the magnetic in-plane anisotropy show no
dependence on the film thickness. However, the strength of the magnetocrystalline anisotropy
decreases with increasing film thickness. XPS and XRD measurements have indicated that
the iron buffer layer is completely oxidized during the second growth stage of the magnetite.
The small Kerr rotation in the MOKE experiments of the samples with film thicknesses up
to 28 nm confirms this result since a remaining iron film would cause a higher Kerr rotation.
In the last part of this thesis the structural and magnetic properties of a partially oxidized, a
completely oxidized and a metallic iron film are analyzed. The partially oxidized iron film is
a bilayer with a metallic iron film and an iron oxide film. The surface near stoichiometry of
both oxidized iron films correspond to magnetite as proven by XPS. The structural analysis
by XRD reveals that though these magnetite films are crystalline, they have an inhomogeneous
thickness. The magnetization curves of the partially oxidized film (bilayer) measured
by MOKE exhibit a magnetic saturation which is comparable to the magnetic saturation of
the single metallic iron film. However, the coercive field is higher compared to the single
metallic iron film due to the high interface roughnesses. Considering the coercive field as a
function of the sample rotation α the bilayer exhibits a fourfold anisotropy with eight maxima.
However, the angular dependence of the magnetic remanence features a simple fourfold
anisotropy with easy axes in h110i directions of MgO(001). Vector MOKE analysis displays
that the magnetic reversal processes of the bilayer are similar to single metallic iron films.
Thus, the bilayer exhibits mostly the magnetic properties of a single iron film. The bilayer
has the same magnetic easy axis and a similar magnetic saturation. The magnetic easy axis
of the magnetic in-plane anisotropy of the completely oxidized iron film is rotated by 45◦
compared to magnetite films grown directly on MgO as already observed in Ref. [148]. The
completely oxidized iron film exhibits also a significantly increased coercive field due to high
surface roughness.
A magneto-dynamic investigation of the exchange-coupling of the Fe3O4/Fe bilayer system
was carried out to yield all relevant magnetic parameters, such as anisotropies, as well as the
coupling constant J1. Here, also a complex fourfold anisotropy was observed, which might
be due to a coupling of a perpendicular spin-wave mode in the magnetite layer with the
acoustical coupling mode. We have also successfully calculated the angular dependence of
the resonance field of all films using the eighth order of the magnetocrystalline anisotropy.
Although we have applied many measurement methods, we have found no explanation for the
complex fourfold angular dependence of the coercive field of the bilayer. Nevertheless, this
bilayer provides interesting properties for application in MTJs due to its enhanced magnetic
properties like complex fourfold magnetic anisotropy and higher coercive field and remanence.
All in all, we have shown that the structural and magnetic properties of magnetite films are
strongly influenced by interlayers between film and substrate. While magnetite films directly
deposited on MgO exhibit a homogeneous film thickness, both NiO interlayers with a thickness
above 24 nm and initially grown iron films deteriorate the structural quality of the on top
grown magnetite films. In addition, the magnetic fourfold anisotropy is rotated by 45◦ in comparison
to magnetite films grown directly on MgO for the structurally disturbed magnetite
on iron pre-covered MgO substrates. Here, further investigations are necessary to understand why this anisotropy rotation occurs and how we can improve the structural quality of
magnetite on iron and NiO. The growth of magnetite by oxidizing previously deposited iron
films leads to crystalline magnetite films but with inhomogeneous film thicknesses. In case
of a Fe3O4/Fe bilayer, the magnetic properties are drastically changed due to the magnetic
coupling between the iron and the magnetite film.

Identiferoai:union.ndltd.org:uni-osnabrueck.de/oai:repositorium.ub.uni-osnabrueck.de:urn:nbn:de:gbv:700-2017012715293
Date27 January 2017
CreatorsSchemme, Tobias
ContributorsProf. Dr. Joachim Wollschläger, Prof. Dr. Heinz-Jürgen Steinhoff
Source SetsUniversität Osnabrück
LanguageEnglish
Detected LanguageEnglish
Typedoc-type:doctoralThesis
Formatapplication/zip, application/pdf
RightsNamensnennung - Weitergabe unter gleichen Bedingungen 3.0 Unported, http://creativecommons.org/licenses/by-sa/3.0/

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