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Register a new userNanosized superparamagnetic precipitates in cobalt-doped ZnO
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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 often 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.
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A comprehensive study of pulsed nitriding in AISI H13 tool steel at low temperature (400{deg}C) is reported for several durations. X-ray diffraction results reveal that a nitrogen enriched compound (Epsilon-Fe2-3N, iron nitride) builds up on the surface within the first process hour despite the low process temperature. Beneath the surface, X-ray Wavelength Dispersive Spectroscopy (WDS) in a Scanning Electron Microscope (SEM) indicates relatively higher nitrogen concentrations (up to 12 at.%) within the diffusion layer while microscopic nitrides are not formed and existing carbides are not dissolved. Moreover, in the diffusion layer, nitrogen is found to be dispersed in the matrix and forming nanosized precipitates. The small coherent precipitates are observed by High-Resolution Transmission Electron Microscopy (HR-TEM) while the presence of nitrogen is confirmed by electron energy loss spectroscopy (EELS). Hardness tests show that the material hardness increases linearly with the nitrogen concentration, reaching up to 14.5 GPa in the surface while the Young Modulus remains essentially unaffected. Indeed, the original steel microstructure is well preserved even in the nitrogen diffusion layer. Nitrogen profiles show a case depth of about ~43 microns after nine hours of nitriding process. These results indicate that pulsed plasma nitriding is highly efficient even at such low temperatures and that at this process temperature it is possible to form thick and hard nitrided layers with satisfactory mechanical properties. This process can be particularly interesting to enhance the surface hardness of tool steels without exposing the workpiece to high temperatures and altering its bulk microstructure.
Long needle-shaped single crystals of Zn1-xCoxO were grown at low temperatures using a molten salt solvent technique, up to x=0.10. The conduction process at low temperatures is determined to be by Mott variable range hopping. Both pristine and cobalt doped crystals clearly exhibit a crossover from negative to positive magnetoresistance as the temperature is decreased. The positive magnetoresistance of the Zn1-xCoxO single crystals increases with increased Co concentration and reaches up to 20% at low temperatures (2.5 K) and high fields (>1 T). SQUID magnetometry confirms that the Zn1-xCoxO crystals are predominantly paramagnetic in nature and the magnetic response is independent of Co concentration. The results indicate that cobalt doping of single crystalline ZnO introduces localized electronic states and isolated Co2+ ions into the host matrix, but that the magnetotransport and magnetic properties are decoupled.
Based on density functional theory calculations, we systematically investigate the behaviors of a H atom in Ag-doped ZnO, involving the preference sites, diffusion behaviors, the electronic structures and vibrational properties. We find that a H atom can migrate to the doped Ag to form a Ag-H complex by overcoming energy barriers of 0.3 - 1.0 eV. The lowest-energy site for H location is the bond center of a Ag-O in the basal plane. Moreover, H can migrate between this site and its equivalent sites with energy cost of less than 0.5 eV. In contrast, dissociation of such a Ag-H complex needs energy of about 1.1 - 1.3 eV. This implies that the Ag-H complexes can commonly exist in the Ag-doped ZnO, which have a negative effect on the desirable p-type carrier concentrations of Ag-doped ZnO. In addition, based on the frozen phonon calculation, the vibrational properties of ZnO with a Ag-H complex are predicted. Some new vibrational modes associated with the Ag-H complex present in the vibrational spectrum of the system.
We calculate the magnetic interactions between two nearest neighbor substitutional magnetic ions (Co or Mn) in ZnO by means of density functional theory and compare it with the available experimental data. Using the local spin density approximation we find a coexistence of ferro- and antiferromagnetic couplings for ZnO:Co, in contrast to experiment. For ZnO:Mn both couplings are antiferromagnetic but deviate quantitatively from measurement. That points to the necessity to account better for the strong electron correlation at the transition ion site which we have done by applying the LSDA+U method. We show that we have to distinguish two different nearest neighbor exchange integrals for the two systems in question which are all antiferromagnetic with values between -1.0 and -2.0 meV in reasonable agreement with experiment.
Fe-doped ZnO nanocrystals are successfully synthesized and structurally characterized by using x-ray diffraction and transmission electron microscopy. Magnetization measurements on the same system reveal a ferromagnetic to paramagnetic transition temperature > 450 K with a low-temperature transition from ferromagnetic to spin-glass state due to canting of the disordered surface spins in the nanoparticle system. Local magnetic probes like EPR and Mossbauer indicate the presence of Fe in both valence states Fe2+ and Fe3+. We argue that the presence of Fe3+ is due to the possible hole doping in the system by cation (Zn) vacancies. In a successive ab-initio electronic structure calculation, the effects of defects (e.g. O- and Zn-vacancy) on the nature and origin of ferromagnetism are investigated for Fe-doped ZnO system. Electronic structure calculations suggest hole doping (Zn-vacancy) to be more effective to stabilize ferromagnetism in Fe doped ZnO and our results are consistent with the experimental signature of hole doping in the ferromagnetic Fe doped ZnO samples.
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