Title: Optical and magneto-optical spectroscopy of materials with antiferro- magnetic interaction Author: Bc. Katarína Križanová Department: Institute of Physics of Charles University Supervisor: RNDr. Jakub Zázvorka, Ph.D., Institute of Physics of Charles University Abstract: One of the goals of spintronic research is the efficient external con- trol of magnetic moment. Non-collinear antiferromagnets in the antiperovskite structure, such as Mn3NiN, show a piezomagnetic effect that can be used to utilize these materials in applications. In the strain free state, the material ex- hibit zero net magnetic moment. Using strain induced by a lattice constant mismatch between the thin layer and a substrate on which the thin film is applied on a non-zero net magnetic moment can be registered. Magneto-optical Kerr effect spectroscopy is used to investigate the non-collinear magnetic thin films. The effect of two substrate layers with resulting opposite sign of strain influencing the magnetic ordering of the antiperovskite material is studied with respect to sample temperature. Results show comparable spectral dependence with opposite sign of the Kerr effect caused by the opposite direc- tion of net magnetization moments. Ellipsometry measurements depending on sample orientation are performed to study the material...

Spintronics is a rapidly growing research field due to scalability, integrablility within existing VLSI architecture, significantly reduced switching energy and latency while maintaining stable bit orientation (Spin-up, Spin-down). For the first time sub-5nm Spin Transfer Torque –Magnetic Tunneling Junctions (STT-MTJ) were investigated utilizing various Integrated Circuit (IC) fabrication techniques to evaluate novel concepts in logic switches. Tunneling Magnetoresistance (TMR) was measured in STT-MTJ stacks of Ta/CoFeB/MgO/CoFeB/Ta with differing diameter ferrimagnetic CoFe2O4 nanoparticles (10nm, 4nm and 2nm) embedded in the MgO layer. MR was detected in the 2nm and 4nm particle devices and demonstrated evidence of single electron transport. Tri-layer STT-MTJ devices were fabricated using a thin film stack of Ta/Ru/Ta/CoFeB(M1)/MgO/CoFeB(M2)/MgO/CoFeB(M3)/Ta. The overall diameter of the stack was reduced to sub-20nm using Focused Ion Beam (FIB) to mill away extra material. The coercivities of the ferrimagnetic CoFeB layers were modified during thin film deposition by altering sputter conditions. Field Applied- Magnetic Force Microscopy (FA-MFM) was used to detect four different magnetic intensities corresponding to three discreet resistances in the singly addressed device, making this architecture a candidate for neuromorphic computational applications. Lastly a lithographic-less architecture was developed to mass fabricate and electo-mechanically probe multi-layered, single point, sub-5nm particle based STT-MTJ devices using off-the-shelf anodized nanoporous alumina. Once fabricated, the devices were probed to measure their IV characteristics and magnetoresistance (MR). The unprecedented MR changes on the order of 50,000% at room temperature suggest quantum mechanical behavior.

Spintronics is a research field that focuses on the manipulation of the quantum mechanical spin of charge carriers in solid state materials for future technological applications. Creating large spin currents with large relaxation times is sought after in the field of spintronics which may be aided by combining spintronics with superconductivity. This thesis provides a phenomological study of the effective change in ferromagnetic resonance linewidth, by dynamical spin injection into a permalloy-copper-niobium tri-layer in the superconducting state. The ferromagetic resonance linewidth was measured from 2-14 K. It was observed that there was a change in the behavior of the resonance as well as a change in the linewidth from the between 6-8 K. An observed change in the resonance field, Hr, shows a clear non monotonic behavior as a function of temperature below 7-8 K. The decrease in linewidth was attributed to the suppression of the spin sinking mechanisms due to the superconducting state of niobium.

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Transport of spin angular momentum (spin currents) in magnetic thin films is important for non-volatile spin-based memory devices and other emerging information technology applications. It is especially important to understand how a spin current propagates across interfaces and how a spin current interacts with magnetic moments. The great interest in devices based on ferromagnetic metals generated intensive theoretical and experimental studies on the basic physics of spin currents for the last few decades. Of particular interest recently is the so-called "pure" electronic spin current, which is carried by electrons and yet unaccompanied by net charge flow, in part because of the prospect of transporting spin with minimal Joule heating. However, in contrast to ferromagnetic metals, spin transport in antiferromagnetic metals, which are promising materials for next-generation magnetic information technology, is not well understood yet. This dissertation addresses the mechanisms of transport by pure spin current in thin-film multilayers incorporating metals with antiferromagnetic order. We focus on two specific materials: (1) CoGd alloys with ferrimagnetic sublattices, which resemble antiferromagnets near the compensation composition, and (2) elemental antiferromagnetic Cr, which can be grown as epitaxial films and hence serve as a model system material. For both the CoGd and Cr studies, spin-valve-like structures of NiFe/Cu/CoGd and NiFe/Cu/Cr/CoFe are prepared to conduct ferromagnetic resonance spin pumping experiments. Precessing magnetization in the NiFe "spin source" pumps a transverse spin current to the adjacent layers. We measure the loss of the spin angular momentum in the "spin sink" layer by measuring the broadening of the resonance linewidth, i.e., the non-local damping enhancement, of the spin source. The antiparallel magnetic moments of Co and Gd sublattices partially cancel out the dephasing of a transverse spin current, thereby resulting in a long spin dephasing length of ≈ 5-6 nm near the magnetic compensation point. We find evidence that the spin current interacts somewhat more strongly with the itinerant transition-metal Co magnetism than the localized rare-earth-metal Gd magnetism in the CoGd alloy. We also examine spin transport via structurally clean antiferromagnetic Cr, epitaxially grown with BCC crystal order. We observe strong spin reflection at the Cu/Cr interface, which is surprising considering that thin layers of Cu and Cr individually are transparent to spin currents carried by electrons. Further, our results indicate other combinations of electrically conductive elemental metals (e.g., Cu/V) can form effective spin-reflecting interfaces. Overall, this thesis advances the basic understanding of spin transport in metallic thin films with and without magnetic order, which can aid the development of next generations of efficient spintronic devices. This work was supported in part by the National Science Foundation, Grant No. DMR-2003914. / Doctor of Philosophy / Manipulation of electronic flow, i.e., net charge flow, underlies modern electronic devices such as computers, mobile phones, and electric cars. However, the conventional charge transport inevitably results in wasted energy, due to resistive (Joule) heating in the devices. A new research area which uses the electron's spin has recently emerged, namely spintronics. Spintronics uses the spin of electrons rather than just the charge, thereby reducing the dependence on charge flow. The flow of spin angular momentum carried by electrons, i.e., "electronic spin current," underpins numerous phenomena in condensed matter physics. An important example is switching and excitation of magnetic order driven electrically by spin current rather than external magnetic field. Spin currents can interact not only with ferromagnetic order consisting of parallel magnetic moments – but also with antiferromagnetic order consisting of alternating magnetic moments that cancel the net magnetization of the material. Indeed, experiments from the last few years demonstrate the ability to rotate antiferromagnetic order (a.k.a. Néel vector) by spin current, which offers new physics not achievable in ferromagnets, such as ultrafast spin dynamics in the THz regime and superfluid spin transport analogous to superconducting electronic transport. However, interaction of a spin current with antiferromagnetic order is not well understood yet. The aim of this thesis is to build a better understanding of spin currents in antiferromagnetic metals. Specifically, we experimentally study basic spin-current physics in a ferrimagnet (CoGd) and an antiferromagnet (Cr). We choose CoGd because adjusting its chemical composition allows us to easily tune its magnetism from ferromagnet-like (uncompensated magnetization) to antiferromagnet-like (compensated magnetization). In antiferromagnet-like CoGd, we find that the oppositely oriented Co and Gd magnetic moments partially cancel the scrambling (dephasing) of spins, so that the spin current is able to propagate over a longer distance - about 3-4 times more than in ferromagnetic metals. The mechanisms behind the longer spin propagation is somewhat akin to the spin "rephasing" technique for lengthening the lifetime of spin-based qubits for quantum computers, but what is remarkable is that we observe this effect in rather disordered magnetic alloys at room temperature. In the other major project of this thesis, we investigate spin transport through multilayers that contain Cr, a structurally and chemically clean antiferromagnetic material. We find that Cr by itself is a good spin transmitter, i.e., effectively allowing a pure spin current to pass through. Surprisingly, when Cr and Cu (another good spin transmitter) are stacked together, we observe strong reflection of a pure spin current at the interface of Cr and Cu. We find that the antiferromagnetic order in Cr is not responsible for this peculiar spin reflection and that other pairs of spin-transmitting metals (for example, V and Cu) can form spin-reflecting interfaces as well. Our work shows an interesting example of "emergent" phenomena where the interface behaves in a way that is not intuitively expected from the properties of the constituent materials. The basic scientific findings from this thesis may help the development of more efficient information-technology devices that run on spin currents.

This thesis describes a research of suppression of superconducting gap in a superconducting island of a Ferromagnetic-Superconducting-Ferromagnetic Single-Electron-Transistor due to the fringing magnetic fields produced by the ferromagnetic leads. The devices are working below the critical temperature of the superconducting gap. A model is proposed to explain how the fringing magnetic field produced by the leads is strong enough to suppress the superconducting gap. The peak of the fringing magnetic field produced by one lead reaches 5000 oe. It is observed an inverse tunneling magneto resistance during the suppression of the superconducting gap, obtaining a maximum absolute value 500 times greater than the TMR in the normal state where the efficiency of the spin injection is low. It is concluded that the suppression of the superconducting gap is due to fringing magnetic field and not to the spin accumulation because the low efficiency of the spin injection. It is suggested a new geometry to reduce the effect of the fringing magnetic field so it can be obtained a suppression of the superconductivity due to the spin accumulation. It is described the qualitatively behavior of the IV characteristic when the suppression of the superconductivity is due to spin accumulation.

This thesis consists of three distinct components: (1) a test of Slocnzewski's theory of spin-transfer torque using the Boltzmann equation, (2) a comparison of macrospin models of spin-transfer dynamics in spin valves with experimental data, and (3) a study of spin-transfer torque in continuously variable magnetization. Slonczewski developed a simple circuit theory for spin-transfer torque in spin valves with thin spacer layer. We developed a numerical method to calculate the spin-transfer torque in a spin valve using Boltzmann equation. In almost all realistic cases, the circuit theory predictions agree well with the Boltzmann equation results. To gain a better understanding of experimental results for spin valve systems, current-induced magnetization dynamics for a spin valve are studied using a single-domain approximation and a generalized Landau-Lifshitz-Gilbert equation. Many features of the experiment were reproduced by the simulations. However, there are two significant discrepancies: the current dependence of the magnetization precession frequency, and the presence and/or absence of a microwave quiet magnetic phase with a distinct magnetoresistance signature. Spin-transfer effects in systems with continuously varying magnetization also have attracted much attention. One key question is under what condition is the spin current adiabatic, i.e., aligned to the local magnetization. Both quantum and semi-classical calculations of the spin current and spin-transfer torque are done in a free-electron Stoner model. The calculation shows that, in the adiabatic limit, the spin current aligns to the local magnetization while the spin density does not. The reason is found in an effective field produced by the gradient of the magnetization in the wall. Non-adiabatic effects arise for short domain walls, but their magnitude decreases exponentially as the wall width increases.

In this thesis, we describe the research in which we use metallic nanoparticles to explore spin-dependent electron transport at nanometer scale. Nanoscale samples were fabricated by using a state of the art electron beam lithography and shadow evaporation technique. We have investigated spin relaxation and decoherence in metallic grains as a function of bias voltage and magnetic field at low temperatures (down to ∼ 30mK). At low temperatures, the discrete energy levels within a metallic nanoparticle provides a new means to study the physics of the spin-polarized electron tunneling. We describe measurements of spin-polarized tunneling via discrete energy levels of single Aluminum grain. Spin polarized current saturates quickly as a function of bias voltage, which demonstrates that the ground state and the lowest excited states carry spin polarized current. The ratio of electron-spin relaxation time (T1) to the electron-phonon relaxation rate is in quantitative agreement with the Elliot-Yafet scaling, an evidence that spin-relaxation in Al grains is driven by the spin-orbit interaction. The spin-relaxation time of the low-lying excited states is T1 ¡Ö 0.7 µs and 0.1 µs in two samples, showing that electron spin in a metallic grain could be a potential candidate for quantum information research. We also present measurements of mesoscopic resistance fluctuations in cobalt nanoparticles at low temperature and study how the fluctuations with bias voltage, bias fingerprints, respond to magnetization-reversal processes. Bias fingerprints rearrange when domains are nucleated or annihilated. The domain wall causes an electron wave function-phase shift of ∼ 5 ¦Ð. The phase shift is not caused by the Aharonov-Bohm effect; we explain how it arises from the mistracking effect, where electron spins lag in orientation with respect to the moments inside the domain wall. The dephasing length at low temperatures is only 30 nm, which is attributed to the large magnetocrystalline anisotropy in Co. xi

The growth of Co (0001) films and Cr2O3 (0001)/Co (0001) has been investigated using surface analysis methods. Such films are of potential importance for a variety of spintronics applications. Co films were directly deposited on commercial Al2O3 (0001) substrates by magnetron sputter deposition or by molecular beam epitaxy (MBE), with thicknesses of ~1000Å or 30Å, respectively. Low Energy Electron Diffraction (LEED) shows hexagonal (1x1) pattern for expected epitaxial films grown at 800 K to ensure the hexagonally close-packed structure. X-ray photoemission spectroscopy (XPS) indicates the metallic cobalt binding energy for Co (2p3/2) peak, which is at 778.1eV. Atomic force microscopy (AFM) indicates the root mean square (rms) roughness of Co films has been dramatically reduced from 10 nm to 0.6 nm by optimization of experiment parameters, especially Ar pressure during plasma deposition. Ultrathin Cr2O3 films (10 to 25 Å) have been successfully fabricated on 1000Å Co (0001) films by MBE. LEED data indicate Cr2O3 has C6v symmetry and bifurcated spots from Co to Cr2O3 with Cr2O3 thickness less than 6 Å. XPS indicates the binding energy of Cr 2p(3/2) is at 576.6eV which is metallic oxide peak. XPS also shows the growth of Cr2O3 on Co (0001) form a thin Cobalt oxide interface, which is stable after exposure to ambient and 1000K UHV anneal.