A series of (Zn,Co)O layers with Co contents x up to 40% grown by atomic layer deposition have been investigated. All structures deposited at 160 • C show magnetic properties specific to II-VI dilute magnetic semiconductors with localized spins S = 3/2 coupled by strong but short-range antiferromagnetic interactions resulting in low-temperature spin-glass freezing for x = 0.16 and 0.4. At higher growth temperature (200 • C) metallic Co nanocrystals precipitate in two locations giving rise to two different magnetic responses: (i) a superparamagnetic contribution coming from volume disperse nanocrystals; (ii) a ferromagneticlike behavior brought about by nanocrystals residing at the (Zn,Co)O/substrate interface. It is shown that the dipolar coupling within the interfacial two-dimensional dense dispersion of nanocrystals is responsible for the ferromagneticlike behavior.
SummaryZinc oxide nanopowders doped with 1–15 mol % cobalt were produced by the microwave solvothermal synthesis (MSS) technique. The obtained nanoparticles were annealed at 800 °C in nitrogen (99.999%) and in synthetic air. The material nanostructure was investigated by means of the following techniques: X-ray diffraction (XRD), helium pycnometry density, specific surface area (SSA), inductively coupled plasma optical emission spectrometry (ICP-OES), extended X-ray absorption fine structure (EXAFS) spectroscopy, scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDS) and with magnetometry using superconducting quantum interference device (SQUID). Irrespective of the Co content, nanoparticles in their initial state present a similar morphology. They are composed of loosely agglomerated spherical particles with wurtzite-type crystal structure with crystallites of a mean size of 30 nm. Annealing to temperatures of up to 800 °C induced the growth of crystallites up to a maximum of 2 μm in diameter. For samples annealed in high purity nitrogen, the precipitation of metallic α-Co was detected for a Co content of 5 mol % or more. For samples annealed in synthetic air, no change of phase structure was detected, except for precipitation of Co3O4 for a Co content of 15 mol %. The results of the magentometry investigation indicated that all as-synthesized samples displayed paramagnetic properties with a contribution of anti-ferromagnetic coupling of Co–Co pairs. After annealing in synthetic air, the samples remained paramagnetic and samples annealed under nitrogen flow showed a magnetic response under the influences of a magnetic field, likely related to the precipitation of metallic Co in nanoparticles.
We demonstrate that room temperature ferromagnetic response (RT FR) of ZnCoO
films grown at low temperature by the Atomic layer Deposition (ALD) method is
due to Co metal accumulations at the ZnCoO/substrate interface region. The
accumulated experimental evi evidences allow us to reject several other
explanations of this effect in our samples, despite the fact that some of them
are likely to be responsible for the low temperature FM in this class of the
material.Comment: 12 pages, 7 figures, 20 reference
We demonstrate that the atomic layer deposition (ALD) technique has large potential to be widely used in a production of ZnO films for applications in electronic, photovoltaic (PV) and optoelectronic devices. Low growth temperature makes the ALD-grown ZnO films suitable for construction of various semiconductor/organic material hybrid structures. This opens possibilities of construction of novel devices based on very cheap organic materials. This includes organic light emitting diodes and PV cells of the third generation, as discussed in the present work.
A series of (Zn,Co)O layers with Co contents x up to 40% grown by atomic layer deposition have been investigated. All structures deposited at 160• C show magnetic properties specific to II-VI dilute magnetic semiconductors with localized spins S = 3/2 coupled by strong but short-range antiferromagnetic interactions resulting in low-temperature spin-glass freezing for x = 0.16 and 0.4. At higher growth temperature (200• C) metallic Co nanocrystals precipitate in two locations giving rise to two different magnetic responses: (i) a superparamagnetic contribution coming from volume disperse nanocrystals; (ii) a ferromagneticlike behavior brought about by nanocrystals residing at the (Zn,Co)O/substrate interface. It is shown that the dipolar coupling within the interfacial two-dimensional dense dispersion of nanocrystals is responsible for the ferromagneticlike behavior.
Despite many efforts the origin of a ferromagnetic (FM) response in ZnMnO and ZnCoO is still not clear. Magnetic investigations of our samples, not discussed here, show that the room temperature FM response is observed only in alloys with a non-uniform Mn or Co distribution. Thus, the control of their distribution is crucial for explanation of contradicted magnetic properties of ZnCoO and ZnMnO reported till now. In the present review we discuss advantages of the Atomic Layer Deposition (ALD) growth method, which enables us to control uniformity of ZnMnO and ZnCoO alloys. Properties of ZnO, ZnMnO and ZnCoO films grown by the ALD are discussed.
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