We show spin lifetimes of 12.6 ns and spin diffusion lengths as long as 30.5 µm in single layer graphene non-local spin transport devices at room temperature. This is accomplished by the fabrication of Co/MgO-electrodes on a Si/SiO2 substrate and the subsequent dry transfer of a graphenehBN-stack on top of this electrode structure where a large hBN flake is needed in order to diminish the ingress of solvents along the hBN-to-substrate interface. Interestingly, long spin lifetimes are observed despite the fact that both conductive scanning force microscopy and contact resistance measurements reveal the existence of conducting pinholes throughout the MgO spin injection/detection barriers. The observed enhancement of the spin lifetime in single layer graphene by a factor of 6 compared to previous devices exceeds current models of contact-induced spin relaxation which paves the way towards probing intrinsic spin properties of graphene.

Recently, it has been shown that oxide barriers in graphene-based non-local spinvalve structures can be the bottleneck for spin transport. The barriers may cause spin dephasing during or right after electrical spin injection which limit spin transport parameters such as the spin lifetime of the whole device. An important task is to evaluate the quality of the oxide barriers of both spin injection and detection contacts in a fabricated device. To address this issue, we discuss the influence of spatially inhomogeneous oxide barriers and especially conducting pinholes within the barrier on the background signal in non-local measurements of graphene/MgO/Co spinvalve devices. By both simulations and reference measurements on devices with nonferromagnetic electrodes, we demonstrate that the background signal can be caused by inhomogeneous current flow through the oxide barriers. As a main result, we demonstrate the existence of charge accumulation next to the actual spin accumulation signal in non-local voltage measurements, which can be explained by a redistribution of charge carriers by a perpendicular magnetic field similar to the classical Hall effect. Furthermore, we present systematic studies on the phase of the low frequency non-local ac voltage signal which is measured in non-local spin measurements when applying ac lock-in techniques. This phase has so far widely been neglected in the analysis of non-local spin transport. We demonstrate that this phase is another hallmark of the homogeneity of the MgO spin injection and detection barriers. We link backgate dependent changes of the phase to the interplay between the capacitance of the oxide barrier to the quantum capacitance of graphene.

In this work an alternate pathway is demonstrated to form ultrathin cobalt ferrite (Co x Fe 3−x O 4) films by interdiffusion of Fe 3 O 4 /CoO bilayers. Bilayer samples with different Fe 3 O 4 /CoO thickness ratios have been prepared by reactive molecular beam epitaxy on Nb-doped SrTiO 3 (001) substrates to obtain cobalt ferrite films of varied stoichiometry. Subsequently, oxygen-assisted postdeposition annealing experiments for consecutive temperature steps between 300 • C and 600 • C have been conducted monitoring the interdiffusion process by means of high-resolution x-ray reflectivity, soft and angle-resolved hard x-ray photoelectron, and x-ray absorption spectroscopy. Magnetic properties were characterized using superconducting quantum interference device magnetometry. The interdiffusion process starts from 300 • C annealing temperature and is completed for temperatures above 500 • C. For completely interdiffused films with Co:Fe ratios larger than 0.84:2 a thin segregated CoO layer on top of the ferrite is formed. This CoO segregation is attributed to surface and interface effects. In addition, multiplet calculations of x-ray absorption spectra are performed to determine the occupancy of different sublattices. These results are correlated with the magnetic properties of the ferrite films. A stoichiometric CoFe 2 O 4 film with partial inversion has been formed exhibiting homogeneously distributed Co 2+ and mainly Fe 3+ valence states if the initial Co:Fe content is 1.09:2. Thus, for the formation of stoichiometric cobalt ferrite by the proposed postdeposition annealing technique an initial Co excess has to be provided as the formation of a top CoO layer is inevitable.

In order to explore an alternative pathway to prepare ultrathin CoFe2O4 films, epitaxial CoO/Fe3O4 bilayers with varying film thickness of the CoO film were grown on Nb-doped SrTiO3(001) substrates via reactive molecular beam epitaxy. Thereafter, cobalt ferrite films with varying stoichiometry were prepared by post-deposition annealing at different temperatures. The thermally mediated interdiffusion resulted in the formation of vertical compressive and lateral tensile strained Co x Fe3 – x O4 films (x = 0.6 – 1.4) with homogeneous distribution of Fe and Co cations for each film. The chemical and electronic variations after each annealing step were studied by means of soft and hard X-ray photoelectron spectroscopy. The homogeneity of the cation distributions in the films were additionally verified after the last annealing step by angle-resolved hard X-ray photoelectron spectroscopy. For the cobalt ferrite film with x = 1.4, an additional crystallographic phase of Co1 – y Fe y O was observed by (grazing incidence) X-ray diffraction measurements after annealing at 600 °C. X-ray reflectivity measurements were performed to determine the film thickness of the formed Co x Fe3 – x O4 films.

A detailed understanding of ultrathin film surface properties is crucial for the proper interpretation of spectroscopic, catalytic, and spin-transport data. We present x-ray magnetic circular dichroism (XMCD) and x-ray resonant magnetic reflectivity (XRMR) measurements on ultrathin Fe 3 O 4 films to obtain magnetic depth profiles for the three resonant energies corresponding to the different cation species Fe 2+ oct , Fe 3+ tet , and Fe 3+ oct located on octahedral and tetrahedral sites of the inverse spinel structure of Fe 3 O 4 . By analyzing the XMCD spectrum of Fe 3 O 4 using multiplet calculations, the resonance energy of each cation species can be isolated. Performing XRMR on these three resonant energies yields magnetic depth profiles that each correspond to one specific cation species. The depth profiles of both kinds of Fe 3+ cations reveal a (3.9 ± 1.0)-Å-thick surface layer of enhanced magnetization, which is likely due to an excess of these ions at the expense of the Fe 2+ oct species in the surface region. The magnetically enhanced Fe 3+ tet layer is additionally shifted about 2.9 ± 0.4 Å farther from the surface than the Fe 3+ oct layer.