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Register a new userImpurity-Ion pair induced high-temperature ferromagnetism in Co-doped ZnO
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Magnetic 3d-ions doped into wide-gap oxides show signatures of room temperature ferromagnetism, although their concentration is two orders of magnitude smaller than that in conventional magnets. The prototype of these exceptional materials is Co-doped ZnO, for which an explanation of the room temperature ferromagnetism is still elusive. Here we demonstrate that magnetism originates from Co2+ oxygen-vacancy pairs with a partially filled level close to the ZnO conduction band minimum. The magnetic interaction between these pairs is sufficiently long-ranged to cause percolation at moderate concentrations. However, magnetically correlated clusters large enough to show hysteresis at room temperature already form below the percolation threshold and explain the current experimental findings. Our work demonstrates that the magnetism in ZnO:Co is entirely governed by intrinsic defects and a phase diagram is presented. This suggests a recipe for tailoring the magnetic properties of spintronics materials by controlling their intrinsic defects.
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The nature of the often reported room temperature ferromagnetism in transition metal doped oxides is still a matter of huge debate. Herein we report on room temperature ferromagnetism in high quality Co-doped ZnO (Zn1-xCoxO) bulk samples synthesized via standard solid-state reaction route. Reference paramagnetic Co-doped ZnO samples with low level of structural defects are subjected to heat treatments in a reductive atmosphere in order to introduce defects in the samples in a controlled way. A detailed structural analysis is carried out in order to characterize the induced defects and their concentration. The magnetometry revealed the coexistence of a paramagnetic and a ferromagnetic phase at room temperature in straight correlation with the structural properties. The saturation magnetization is found to increase with the intensification of the heat treatment, and, therefore, with the increase of the density of induced defects. The magnetic behavior is fully explained in terms of the bound magnetic polaron model. Based on the experimental findings, supported by theoretical calculations, we attribute the origin of the observed defect-induced-ferromagnetism to the ferromagnetic coupling between the Co ions mediated by magnetic polarons due to zinc interstitial defects.
Unexpected ferromagnetism has been observed in carbon doped ZnO films grown by pulsed laser deposition [Phys. Rev. Lett. 99, 127201 (2007)]. In this letter, we introduce carbon into ZnO films by ion implantation. Room temperature ferromagnetism has been observed. Our analysis demonstrates that (1) C-doped ferromagnetic ZnO can be achieved by an alternative method, i.e. ion implantation, and (2) the chemical involvement of carbon in the ferromagnetism is indirectly proven.
We have studied the structural, magnetic and electronic properties of Co-implanted ZnO (0001) films grown on Al2O3 (1120) substrates for different implantation doses and over a wide temperature range. Strong room temperature ferromagnetism is observed with magnetic parameters depending on the cobalt implantation dose. A detailed analysis of the structural and magnetic properties indicates that there are two magnetic phases in Co-implanted ZnO films. One is a ferromagnetic phase due to the formation of long range ferromagnetic ordering between implanted magnetic cobalt ions in the ZnO layer, the second one is a superparamagnetic phase, which occurs due to the formation of metallic cobalt clusters in the Al2O3 substrate. Using x-ray resonant magnetic scattering, the element specific magnetization of cobalt, oxygen and Zn was investigated. Magnetic dichroism was observed at the Co L2,3 edges as well as at the O K edge. In addition, the anomalous Hall effect is also observed, supporting the intrinsic nature of ferromagnetism in Co-implanted ZnO films.
We report on structural, magnetic and electronic properties of Co-implanted TiO2 rutile single crystals for different implantation doses. Strong ferromagnetism at room temperature and above is observed in TiO2 rutile plates after cobalt ion implantation, with magnetic parameters depending on the cobalt implantation dose. While the structural data indicate the presence of metallic cobalt clusters, the multiplet structure of the Co L3 edge in the XAS spectra gives clear evidence for a substitutional Co 2+ state. The detailed analysis of the structural and magnetic properties indicates that there are two magnetic phases in Co-implanted TiO2 plates. One is a ferromagnetic phase due to the formation of long range ferromagnetic ordering between implanted magnetic cobalt ions in the rutile phase, and the second one is a superparamagnetic phase originates from the formation of metallic cobalt clusters in the implanted region. Using x-ray resonant magnetic scattering, the element specific magnetization of cobalt, oxygen and titanium in Co-implanted TiO2 single crystals are investigated. Magnetic dichroism was observed at the Co L edges as well as at the O K edge. The interaction mechanism, which leads to ferromagnetic ordering of substituted cobalt ions in the host matrix, is also discussed.
We studied structural, optical and magnetic properties of high-quality 5 and 15% Co-doped ZnO films grown by plasma-assisted molecular beam epitaxy (MBE) on (0001)-sapphire substrates. Magnetic force microscopy (MFM) and magnetic measurements with SQUID magnetometer show clear ferromagnetic behavior of the films up to room temperature whereas they are antiferromagnetic below 200 K approximately. Temperature dependence of the carrier mobility was determined using Raman line shape analysis of the longitudinal-optical-phonon-plasmon coupled modes. It shows that the microscopic mechanism for ferromagnetic ordering is coupling mediated by free electrons between spins of Co atoms. These results bring insight into a subtle interplay between charge carriers and magnetism in MBE-grown Zn(1-x)CoxO films.
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