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Register a new userDefect Induced Room Temperature Ferromagnetism in High Quality Co-doped ZnO Bulk Samples
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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.
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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.
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 prove a spontaneous magnetization of the oxygen-terminated ZnO (0001) surface by utilizing a multi-code, SIESTA and KKR, first-principles approach, involving both LSDA+U and selfinteraction corrections (SIC) to treat electron correlation effects. Critical temperatures are estimated from Monte Carlo simulations, showing that at and above 300 K the surface is thermodynamically stable and ferromagnetic. The observed half-metallicity and long-range magnetic order originate from the presence of p-holes in the valence band of the oxide. The mechanism is universal in ionic oxides and points to a new route for the design of ferromagnetic low dimensional systems.
Ab initio studies have theoretically predicted room temperature ferromagnetism in crystalline SnO2, ZrO2 and TiO2 doped with non magnetic element from the 1A column as K and Na. Our purpose is to address experimentally the possibility of magnetism in both Sn1-xKxO2 and Sn1-xCaxO2 compounds. The samples have been prepared using equilibrium methods of standard solid state route. Our study has shown that both Sn1-xCaxO2 and Sn1-xKxO2 structure is thermodynamically unstable and leads to a phase separation, as shown by X-ray diffraction and detailed micro-structural analyses with high resolution transmission electron microscopy (TEM). In particular, the crystalline SnO2 grains are surrounded by K-based amorphous phase. In contrast to Ca: SnO2 samples we have obtained a magnetic phase in K: SnO2 ones, but no long range ferromagnetic order. The K: SnO2 samples exhibit a moments of the order of 0.2 {mu}B/K /ion, in contrast to ab-initio calculations which predict 3{mu}B, where K atoms are on the Sn crystallographic site. The apparent contradictions between our experiments and first principle studies are discussed.
Thermal ammonolysis of quasi-two-dimensional (quasi-2D) CoTa2O6 yields the O2-/N3- and anionic vacancy ordered Co2+Ta5+2O6-xN2x/3$Box$x/3 (x $leq$ 0.15) that exhibits a transition from antiferromagnetism to defect engineered above room-temperature ferromagnetism as evidenced by diffraction, spectroscopic and magnetic characterizations. First-principles calculations reveal the origin of ferromagnetism is a particular CoON configuration with N located at Wyckoff position 8j, which breaks mirror symmetry about ab plane. A pressure-induced electronic phase transition is also predicted at around 24.5 GPa, accompanied by insulator-to-metal transition and magnetic moment vanishing.
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