Advanced scanning magnetoresistive microscopy (SMRM) — a robust magnetic imaging and probing technique — is presented. It utilizes conventional recording heads of a hard disk drive as sensors. The spatial resolution of modern tunneling magnetoresistive sensors is nowadays comparable with more commonly used magnetic force microscopes. Important advantages of SMRM are the ability to detect pure magnetic signals directly proportional to the out-of-plane magnetic stray field, negligible sensor stray fields, and the ability to apply local bipolar magnetic field pulses up to 10 kOe with bandwidths from DC up to 1 GHz. The performance assessment of this method and corresponding best practices are discussed in the first section of this work. An application example of SMRM, the study on chemically ordered L10 FePt is presented in a second section. A constructed heater unit of SMRM opens the path to investigate temperature-dependent magnetic properties of the medium by recording and imaging at elevated temperatures. L10 FePt is one of the most promising materials to reach limits in storage density of future magnetic recording devices based on heat-assisted magnetic recording (HAMR). In order to be implemented in an actual recording scheme, the medium Curie temperature should be lowered. This will reduce the power requirements, and hence, wear and tear on a heat source — integrated plasmonic antenna. It is expected that the exchange coupling of FePt to thin Fe layers provides high saturation magnetization and elevated Curie temperature of the composite. The addition of Cu allows adjusting the magnetic properties such as perpendicular magnetic anisotropy, coercivity, saturation magnetization, and Curie temperature. This should lead to a lowering of the switching field of the hard magnetic FeCuPt layer and a reduction of thermally induced recording errors. In this regard, the influence of the Fe layer thickness on the switching behavior of the hard layer was investigated, revealing a strong reduction for Fe layer thicknesses larger than the exchange length of Fe. The recording performance of single-layer and bilayer structures was studied by SMRM roll-off curves and histogram methods at temperatures up to 180 °C In the last section of this work, SMRM advantages are demonstrated by various experiments on a two-dimensional magnetic vortex lattice. Magnetic vortex is a peculiar complex magnetization configuration which typically appears in a soft magnetic structured materials. It consists of two coupled sub-systems: the core, where magnetization vector points perpendicular to the structure plane, and the curling magnetization where magnetic flux is rotating in-plane. The unique properties of a magnetic vortex making it an object of a great research and technological interest for spintronic applications in sensorics or data storage. Manipulation of the vortex core as well as the rotation sense by applying a local field pulse is shown. A spatially resolved switching map reveals a significant "write window" where vortex cores can be addressed correctly. Moreover, the external in-plane magnet extension unit allow analyzing the magnetic vortex rotational sense which is extremely practical for magnetic coupling investigations of magnetic coupling phenomena.

The work presented in this thesis encompasses the design, development, realization and testing of novel magnetoelectric thin film elements that do not rely on ferromagnets, but are based entirely on magnetoelectric antiferromagnets such as Cr2O3. Thin film spintronic elements, and in particular magnetoelectric transducers, are crucial building blocks of high efficiency data processing schemes that could complement conventional electronic data processing in the future. Recent developments in magnetoelectrics have revealed, that exchange biased systems are ill-suited to electric field induced switching of magnetization due to the strong coupling of their ferromagnetic layer to magnetic fields. Therefore, ferromagnet-free magnetoelectric elements are proposed here in an effort to mitigate the practical problems associated with existing exchange biased magnetoelectric elements. This goal is achieved by establishing an all-electric read-out method for the antiferromagnetic order parameter of thin films, which allows to omit the ferromagnet from conventional exchange biased magnetoelectric elements. The resulting ferromagnet-free magnetoelectric elements show greatly reduced writing thresholds, enabled operation at room temperature and do not require a pulsed magnetic field, all of which is in contrast to state-of-the-art exchange biased magnetoelectric systems. The novel all-electric read-out method of the magnetic field-invariant magnetization of antiferromagnets, so-called spinning-current anomalous Hall magnetometry, can be widely employed in other areas of thin film magnetism. Its high precision and its sensitivity to previously invisible phenomena make it a promising tool for various aspects of thin solid films. Based on this technique, a deep understanding could be generated as to what physical mechanisms drive the antiferromagnetic ordering in thin films of magnetoelectric antiferromagnets. As spinning-current anomalous Hall magnetometry is an integral probe of the magnetic properties in thin films, it offers no intrinsic scale sensitivity. In order to harness its great precision for scale related information, a statistical framework was developed, which links macroscopic measurements with microscopic properties such as the antiferromagnetic domain size.

Advanced scanning magnetoresistive microscopy (SMRM) — a robust magnetic imaging and probing technique — is presented. It utilizes conventional recording heads of a hard disk drive as sensors. The spatial resolution of modern tunneling magnetoresistive sensors is nowadays comparable with more commonly used magnetic force microscopes. Important advantages of SMRM are the ability to detect pure magnetic signals directly proportional to the out-of-plane magnetic stray field, negligible sensor stray fields, and the ability to apply local bipolar magnetic field pulses up to 10 kOe with bandwidths from DC up to 1 GHz. The performance assessment of this method and corresponding best practices are discussed in the first section of this work. An application example of SMRM, the study on chemically ordered L10 FePt is presented in a second section. A constructed heater unit of SMRM opens the path to investigate temperature-dependent magnetic properties of the medium by recording and imaging at elevated temperatures. L10 FePt is one of the most promising materials to reach limits in storage density of future magnetic recording devices based on heat-assisted magnetic recording (HAMR). In order to be implemented in an actual recording scheme, the medium Curie temperature should be lowered. This will reduce the power requirements, and hence, wear and tear on a heat source — integrated plasmonic antenna. It is expected that the exchange coupling of FePt to thin Fe layers provides high saturation magnetization and elevated Curie temperature of the composite. The addition of Cu allows adjusting the magnetic properties such as perpendicular magnetic anisotropy, coercivity, saturation magnetization, and Curie temperature. This should lead to a lowering of the switching field of the hard magnetic FeCuPt layer and a reduction of thermally induced recording errors. In this regard, the influence of the Fe layer thickness on the switching behavior of the hard layer was investigated, revealing a strong reduction for Fe layer thicknesses larger than the exchange length of Fe. The recording performance of single-layer and bilayer structures was studied by SMRM roll-off curves and histogram methods at temperatures up to 180 °C In the last section of this work, SMRM advantages are demonstrated by various experiments on a two-dimensional magnetic vortex lattice. Magnetic vortex is a peculiar complex magnetization configuration which typically appears in a soft magnetic structured materials. It consists of two coupled sub-systems: the core, where magnetization vector points perpendicular to the structure plane, and the curling magnetization where magnetic flux is rotating in-plane. The unique properties of a magnetic vortex making it an object of a great research and technological interest for spintronic applications in sensorics or data storage. Manipulation of the vortex core as well as the rotation sense by applying a local field pulse is shown. A spatially resolved switching map reveals a significant "write window" where vortex cores can be addressed correctly. Moreover, the external in-plane magnet extension unit allow analyzing the magnetic vortex rotational sense which is extremely practical for magnetic coupling investigations of magnetic coupling phenomena.

The work presented in this thesis encompasses the design, development, realization and testing of novel magnetoelectric thin film elements that do not rely on ferromagnets, but are based entirely on magnetoelectric antiferromagnets such as Cr2O3. Thin film spintronic elements, and in particular magnetoelectric transducers, are crucial building blocks of high efficiency data processing schemes that could complement conventional electronic data processing in the future. Recent developments in magnetoelectrics have revealed, that exchange biased systems are ill-suited to electric field induced switching of magnetization due to the strong coupling of their ferromagnetic layer to magnetic fields. Therefore, ferromagnet-free magnetoelectric elements are proposed here in an effort to mitigate the practical problems associated with existing exchange biased magnetoelectric elements. This goal is achieved by establishing an all-electric read-out method for the antiferromagnetic order parameter of thin films, which allows to omit the ferromagnet from conventional exchange biased magnetoelectric elements. The resulting ferromagnet-free magnetoelectric elements show greatly reduced writing thresholds, enabled operation at room temperature and do not require a pulsed magnetic field, all of which is in contrast to state-of-the-art exchange biased magnetoelectric systems. The novel all-electric read-out method of the magnetic field-invariant magnetization of antiferromagnets, so-called spinning-current anomalous Hall magnetometry, can be widely employed in other areas of thin film magnetism. Its high precision and its sensitivity to previously invisible phenomena make it a promising tool for various aspects of thin solid films. Based on this technique, a deep understanding could be generated as to what physical mechanisms drive the antiferromagnetic ordering in thin films of magnetoelectric antiferromagnets. As spinning-current anomalous Hall magnetometry is an integral probe of the magnetic properties in thin films, it offers no intrinsic scale sensitivity. In order to harness its great precision for scale related information, a statistical framework was developed, which links macroscopic measurements with microscopic properties such as the antiferromagnetic domain size.:TABLE OF CONTENTS Abbreviations 9 1 Introduction 11 1.1 Motivation 11 1.2 Objectives 12 1.3 Organization of the thesis 13 2 Background 15 2.1 History of magnetoelectric coupling 15 2.2 Long range magnetic ordering 16 2.2.1 Magnetic order parameter and field susceptibility 17 2.2.2 Magnetic proximity effect 19 2.2.3 Exchange bias 20 2.3 Phenomenology of magnetoelectric coupling 21 2.3.1 The linear magnetoelectric effect 21 2.3.2 Magnetoelectric pressure on the antiferromagnetic order parameter 22 2.3.3 Switching the antiferromagnetic order parameter 23 2.4 Realized magnetoelectric thin film elements 24 2.4.1 BiFeO3/CoFe system 24 2.4.2 Cr2O3/Co/Pt system 25 3 Experimental methods 27 3.1 Development of ferromagnet free magnetoelectric elements 28 3.1.1 The substrate 29 3.1.2 The Cr2O3 bulk and top surface 31 3.1.3 The V2O3 or Pt bottom electrodes 33 3.1.4 Epitaxial relationships 34 3.1.5 The Cr2O3 bottom interface 39 3.1.6 Twinning of Cr2O3 39 3.1.7 Hall crosses and patterning processes 43 3.2 Magnetotransport measurements 44 3.2.1 Hall effects 45 3.2.2 Anomalous Hall effect 46 3.2.3 Magnetoelectric writing 47 3.2.4 All electric read out 49 3.3 The experimental setup 50 3.3.1 Temperature control 50 3.3.2 Magnetic field control 51 4 Spinning-current anomalous Hall magnetometry 53 4.1 Characteristics of the technique 53 4.1.1 Operational principle 53 4.1.2 Advantages 55 4.1.3 Magnetic hysteresis loops and field-invariant magnetization 55 4.1.4 Measurement of field-invariant magnetization 56 4.1.5 Limitations 58 4.2 Application of SCAHM to Cr2O3(0001) thin films 59 4.2.1 Criticality and distribution of the antiferromagnetic phase transition 61 4.2.2 Evaluation of the magnetic proximity effect 64 4.3 SCAHM with thin metallic antiferromagnetic IrMn films 65 4.3.1 [Pt/Co]4/IrMn exchange bias system 65 4.3.2 Isolated antiferromagnetic IrMn thin films 67 5 Magnetoelectric performance 69 5.1 Magnetoelectric field cooling 69 5.2 The gate bias voltage 71 5.3 Isothermal binary magnetoelectric writing in Cr2O3 72 6 Order parameter selection in magnetoelectric antiferromagnets 77 6.1 Uncompensated magnetic moment 77 6.2 Extrinsic causes for broken sublattice equivalence 81 6.3 The V2O3 gate electrode 83 7 Measurement of microscopic properties with an integral probe 87 7.1 Interentity magnetic exchange coupling 87 7.2 Ensemble formalism for the entity size determination 90 7.3 Estimation of the entity sizes 94 7.4 Microscopic confirmation of the ensemble model 97 8 Summary and Outlook 101 8.1 Goal-related achievements 101 8.1.1 All-electric read-out of the AF order parameter 101 8.1.2 Electric field induced writing of the AF order parameter 102 8.2 Further achievements 103 8.2.1 Foreseen impact of SCAHM on thin film magnetism 103 8.2.2 Practical optimization routes of magnetoelectric Cr2O3 systems 104 8.2.3 Theoretical work 105 8.3 Future directions 105 8.3.1 Development of Cr2O3-based magnetoelectric systems 105 8.3.2 Applications of SCAHM 106 References 107 Erklärung 113 Acknowledgements 115 Curriculum Vitae 117 Scientific publications, contributions, patents 119