Title: Materials Optimization and GHz Spin Dynamics of Metallic Ferromagnetic Thin Film Heterostructures
Description: Metallic ferromagnetic (FM) thin film heterostructures play an important role in emerging magnetoelectronic devices, which introduce the spin degree of freedom of electrons into conventional charge-based electronic devices. As the majority of magnetoelectronic devices operate in the GHz frequency range, it is critical to understand the high-frequency magnetization dynamics in these structures. In this thesis, we start with the static magnetic properties of FM thin films and their optimization via the field-sputtering process incorporating a specially designed in-situ electromagnet. We focus on the origins of anisotropy and hysteresis/coercivity in soft magnetic thin films, which are most relevant to magentic susceptibility and power dissipation in applications in the sub-GHz frequency regime, such as magnetic-core integrated inductors. Next we explore GHz magnetization dynamics in thin-film heterostructures, both in semi-infinite samples and confined geometries. All investigations are rooted in the Landau-Lifshitz-Gilbert (LLG) equation, the equation of motion for magnetization.

The phenomenological Gilbert damping parameter in the LLG equation has been interpreted, since the 1970's, in terms of the electrical resistivity. We present the first interpretation of the size effect in Gilbert damping in single metallic FM films based on this electron theory of damping. The LLG equation is intrinsically nonlinear, which provides possibilities for rf signal processing. We analyze the frequency doubling effect at small-angle magnetization precession from the first-order expansion of the LLG equation, and demonstrate second harmonic generation from Ni81 Fe19 (Permalloy) thin film under ferromagnetic resonance (FMR), three orders of magnitude more efficient than in ferrites traditionally used in rf devices. Though the efficiency is less than in semiconductor devices, we provide field- and frequency-selectivity in the second harmonic generation. To address further the relationship between the rf excitation and the magnetization dynamics in systems with higher complexity, such as multilayered thin films consisting of nonmagnetic (NM) and FM layers, we employ the powerful time-resolved x-ray magnetic circular dichroism (TR-XMCD) spectroscopy.

Soft x-rays have element-specific absorption, leading to layer-specific magnetization detection provided the FM layers have distinctive compositions. We discovered that in contrast to what has been routinely assumed, for layer thicknesses well below the skin depth of the EM wave, a significant phase difference exists between the rf magnetic fields Hrf in different FM layers separated by a Cu spacer layer. We propose an analysis based on the distribution of the EM waves in the film stack and substrate to interpret this striking observation. For confined geometries with lateral dimensions in the sub-micron regime, there has been a critical absence of experimental techniques which can image small-amplitude dynamics of these structures. We extend the TR-XMCD technique to scanning transmission x-ray microscopy (STXM), to observe directly the local magnetization dynamics in nanoscale FM thin-film elements, demonstrated at picosecond temporal, 40 nm spatial and less than 6° angular resolution.

The experimental data are compared with our micromagnetic simulations based on the finite element analysis of the time-dependent LLG equation. We resolve standing spin wave modes in nanoscale Ni81 Fe19 thin film ellipses (1000 nm × 500 nm × 20 nm) with clear phase information to distinguish between degenerate eigenmodes with different symmetries for the first time. With the element-specific imaging capability of soft x-rays, spatial resolution up to 15 nm with improved optics, we see great potential for this technique to investigate functional devices with multiple FM layers, and provide insight into the studies of spin injection, manipulation and detection.