During the past years there has been renewed interest in the wide-bandgap II-VI semiconductor ZnO, triggered by promising prospects for spintronic applications. First, ferromagnetism was predicted for dilute magnetic doping. In comprehensive investig
ation of ZnO:Co thin films based on the combined measurement of macroscopic and microscopic properties, we find no evidence for carrier-mediated itinerant ferromagnetism. Phase-pure, crystallographically excellent ZnO:Co is uniformly paramagnetic. Superparamagnetism arises when phase separation or defect formation occurs, due to nanometer-sized metallic precipitates. Other compounds like ZnO:(Li,Ni) and ZnO:Cu do not exhibit indication of ferromagnetism. Second, its small spin-orbit coupling and correspondingly large spin coherence length makes ZnO suitable for transporting or manipulating spins in spintronic devices. From optical pump/optical probe experiments, we find a spin dephasing time of the order of 15 ns at low temperatures which we attribute to electrons bound to Al donors. In all-electrical magnetotransport measurements, we successfully create and detect a spin-polarized ensemble of electrons and transport this spin information across several nanometers. We derive a spin lifetime of 2.6 ns for these itinerant spins at low temperatures, corresponding well to results from an electrical pump/optical probe experiment.
In a recent Letter [Y.M. Lu et al., Phys. Rev. Lett. 110, 147207 (2013)], Lu et al. reported on ferromagneticlike transport properties of thin films of Pt, deposited ex situ via sputtering on the ferrimagnetic insulator Y3Fe5O12. The authors found a
magnetoresistance in Pt displaying a hysteresis corresponding to the coercive field of Y3Fe5O12, consistent with the findings of other groups. While the latter interpreted their data in terms of the recently proposed spin-Hall magnetoresistance, Lu et al. attributed their observation to a magnetic proximity effect. To support this interpretation, they measured the X-ray magnetic circular dichroism (XMCD) at the Pt L2,3 edges from a Pt/Y3Fe5O12 sample with a Pt thickness of 1.5 nm and derived an average induced magnetic moment of 0.054 Bohr magnetons per Pt atom. This is contradictory to the results of our previous comprehensive XMCD study of three different Pt/Y3Fe5O12 samples with Pt thicknesses of 3, 7, and 10 nm from which we identified an upper limit of (0.003 +/- 0.001) Bohr magnetons per Pt [Geprags et al., Appl. Phys. Lett. 101, 262407 (2012), arXiv:1211.0916].
We report on the growth of epitaxial ZnO thin films and ZnO based heterostructures on sapphire substrates by laser molecular beam epitaxy (MBE). We first discuss some recent developments in laser-MBE such as flexible ultra-violet laser beam optics, i
nfrared laser heating systems or the use of atomic oxygen and nitrogen sources, and describe the technical realization of our advanced laser-MBE system. Then we describe the optimization of the deposition parameters for ZnO films such as laser fluence and substrate temperature and the use of buffer layers. The detailed structural characterization by x-ray analysis and transmission electron microscopy shows that epitaxial ZnO thin films with high structural quality can be achieved, as demonstrated by a small out-of-plane and in-plane mosaic spread as well as the absence of rotational domains. We also demonstrate the heteroepitaxial growth of ZnO based multilayers as a prerequisite for spin transport experiments and the realization of spintronic devices. As an example, we show that TiN/Co/ZnO/Ni/Au multilayer stacks can be grown on (0001)-oriented sapphire with good structural quality of all layers and well defined in-plane epitaxial relations.
The wide bandgap semiconductor ZnO is interesting for spintronic applications because of its small spin-orbit coupling implying a large spin coherence length. Utilizing vertical spin valve devices with ferromagnetic electrodes (TiN/Co/ZnO/Ni/Au), we
study the spin-polarized transport across ZnO in all-electrical experiments. The measured magnetoresistance agrees well with the prediction of a two spin channel model with spin-dependent interface resistance. Fitting the data yields spin diffusion lengths of 10.8nm (2K), 10.7nm (10K), and 6.2nm (200K) in ZnO, corresponding to spin lifetimes of 2.6ns (2K), 2.0ns (10K), and 31ps (200K).
The recent study of oxides led to the discovery of several new fascinating physical phenomena. High-temperature superconductivity, colossal magnetoresistance, dilute magnetic doping, or multiferroicity were discovered and investigated in transition-m
etal oxides, representing a prototype class of strongly correlated electronic systems. This development was accompanied by an enormous progress regarding thin film fabrication. Within the past two decades, epitaxial thin films with crystalline quality approaching semiconductor standards became available using laser molecular beam epitaxy. This evolution is reviewed, particularly with emphasis on transition-metal oxide thin films, their versatile physical properties, and their impact on the field of spintronics. First, the physics of ferromagnetic half-metallic oxides, such as the doped manganites, the double perovskites and magnetite is presented together with possible applications based on magnetic tunnel junctions. Second, the wide bandgap semiconductor zinc oxide is discussed particularly with regard to the controversy of dilute magnetic doping with transition-metal ions and the possibility of realizing p-type conductivity. Third, the field of oxide multiferroics is presented with the recent developments in single-phase multiferroic thin film perovskites as well as in composite multiferroic hybrids.
Transition metal oxides show fascinating physical properties such as high temperature superconductivity, ferro- and antiferromagnetism, ferroelectricity or even multiferroicity. The enormous progress in oxide thin film technology allows us to integra
te these materials with semiconducting, normal conducting, dielectric or non-linear optical oxides in complex oxide heterostructures, providing the basis for novel multi-functional materials and various device applications. Here, we report on the combination of ferromagnetic, semiconducting, metallic, and dielectric materials properties in thin films and artificial heterostructures using laser molecular beam epitaxy. We discuss the fabrication and characterization of oxide-based ferromagnetic tunnel junctions, transition metal-doped semiconductors, intrinsic multiferroics, and artificial ferroelectric/ferromagetic heterostructures - the latter allow for the detailed study of strain effects, forming the basis of spin-mechanics. For characterization we use X-ray diffraction, SQUID magnetometry, magnetotransport measurements, and advanced methods of transmission electron microscopy with the goal to correlate macroscopic physical properties with the microstructure of the thin films and heterostructures.
The ferrimagnetic spinel oxide Zn(x)Fe(3-x)O(4) combines high Curie temperature and spin polarization with tunable electrical and magnetic properties, making it a promising functional material for spintronic devices. We have grown epitaxial thin film
s with 0<=x<=0.9 on MgO(001) substrates with excellent structural properties both in pure Ar atmosphere and an Ar/O2 mixture by laser molecular beam epitaxy. We find that the electrical conductivity and the saturation magnetization can be tuned over a wide range during growth. Our extensive characterization of the films provides a clear picture of the underlying physics of this spinel ferrimagnet with antiparallel Fe moments on the A and B sublattice: (i) Zn substitution removes both Fe3+ moments from the A sublattice and itinerant charge carriers from the B sublattice, (ii) growth in finite oxygen partial pressure generates Fe vacancies on the B sublattice also removing itinerant charge carriers, and (iii) application of both Zn substitution and excess oxygen results in a compensation effect as Zn substitution partially removes the Fe vacancies. A decrease (increase) of charge carrier density results in a weakening (strengthening) of double exchange and thereby a decrease (increase) of conductivity and the saturation magnetization. This scenario is confirmed by the observation that the saturation magnetization scales with the longitudinal conductivity. The combination of tailored films with semiconductor materials such as ZnO in multi-functional heterostructures seems to be particularly appealing.
The existence of semiconductors exhibiting long-range ferromagnetic ordering at room temperature still is controversial. One particularly important issue is the presence of secondary magnetic phases such as clusters, segregations, etc... These are of
ten tedious to detect, leading to contradictory interpretations. We show that in our cobalt doped ZnO films grown homoepitaxially on single crystalline ZnO substrates the magnetism unambiguously stems from metallic cobalt nano-inclusions. The magnetic behavior was investigated by SQUID magnetometry, x-ray magnetic circular dichroism, and AC susceptibility measurements. The results were correlated to a detailed microstructural analysis based on high resolution x-ray diffraction, transmission electron microscopy, and electron-spectroscopic imaging. No evidence for carrier mediated ferromagnetic exchange between diluted cobalt moments was found. In contrast, the combined data provide clear evidence that the observed room temperature ferromagnetic-like behavior originates from nanometer sized superparamagnetic metallic cobalt precipitates.
The anomalous Hall effect (AHE) has been studied systematically in the low-conductivity ferromagnetic oxide Fe$_{3-x}$Zn$_x$O$_4$ with $x = 0$, 0.1, and 0.5. We used (001), (110), and (111) oriented epitaxial Fe$_{3-x}$Zn$_x$O$_4$ films grown on MgO
and sapphire substrates in different oxygen partial pressure to analyze the dependence of the AHE on crystallographic orientation, Zn content, strain state, and oxygen deficiency. Despite substantial differences in the magnetic properties and magnitudes of the anomalous Hall conductivity $sigma_{xy}^{rm AHE}$ and the longitudinal conductivity $sigma_{xx}$ over several orders of magnitude, a universal scaling relation $sigma_{xy}^{rm AHE} propto sigma_{xx}^{alpha}$ with $alpha = 1.69 pm 0.08$ was found for all investigated samples. Our results are in agreement with recent theoretical and experimental findings for ferromagnetic metals in the dirty limit, where transport is by metallic conduction. We find the same scaling relation for magnetite, where hopping transport prevails. The fact that this relation is independent of crystallographic orientation, Zn content, strain state, and oxygen deficiency suggests that it is universal and particularly does not depend on the nature of the transport mechanism.
