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Register a new userParamagnetism of the Co sublattice in ferromagnetic Zn$_{1-x}$Co$_{x}$O films
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Using the spectroscopies based upon x-ray absorption, we have studied the structural and magnetic properties of Zn$_{1-x}$Co$_{x}$O films ($x$ = 0.1 and 0.25) produced by reactive magnetron sputtering. These films show ferromagnetism with a Curie temperature $T_{mathrm{C}}$ above room temperature in bulk magnetization measurements. Our results show that the Co atoms are in a divalent state and in tetrahedral coordination, thus substituting Zn in the wurtzite-type structure of ZnO. However, x-ray magnetic circular dichroism at the Co textit{L}$_{2,3}$ edges reveals that the Co 3textit{d} sublattice is paramagnetic at all temperatures down to 2 K, both at the surface and in the bulk of the films. The Co 3textit{d} magnetic moment at room temperature is considerably smaller than that inferred from bulk magnetisation measurements, suggesting that the Co 3textit{d} electrons are not directly at the origin of the observed ferromagnetism.
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The magnetic properties of Zn$_{1-x}$Co$_x$O ($x=0.07$ and 0.10) thin films, which were homo-epitaxially grown on a ZnO(0001) substrates with varying relatively high oxygen pressure, have been investigated using x-ray magnetic circular dichroism (XMCD) at Co $2p$ core-level absorption edge. The line shapes of the absorption spectra are the same in all the films and indicate that the Co$^{2+}$ ions substitute for the Zn sites. The magnetic-field and temperature dependences of the XMCD intensity are consistent with the magnetization measurements, indicating that except for Co there are no additional sources for the magnetic moment, and demonstrate the coexistence of paramagnetic and ferromagnetic components in the homo-epitaxial Zn$_{1-x}$Co$_{x}$O thin films, in contrast to the ferromagnetism in the hetero-epitaxial Zn$_{1-x}$Co$_{x}$O films studied previously. The analysis of the XMCD intensities using the Curie-Weiss law reveals the presence of antiferromagnetic interaction between the paramagnetic Co ions. Missing XMCD intensities and magnetization signals indicate that most of Co ions are non-magnetic probably because they are strongly coupled antiferromagnetically with each other. Annealing in a high vacuum reduces both the paramagnetic and ferromagnetic signals. We attribute the reductions to thermal diffusion and aggregation of Co ions with antiferromagnetic nanoclusters in Zn$_{1-x}$Co$_{x}$O.
Electronic structures of Zn$_{1-x}$Co$_x$O have been investigated using photoemission spectroscopy (PES) and x-ray absorption spectroscopy (XAS). The Co 3d states are found to lie near the top of the O $2p$ valence band, with a peak around $sim 3$ eV binding energy. The Co $2p$ XAS spectrum provides evidence that the Co ions in Zn$_{1-x}$Co$_{x}$O are in the divalent Co$^{2+}$ ($d^7$) states under the tetrahedral symmetry. Our finding indicates that the properly substituted Co ions for Zn sites will not produce the diluted ferromagnetic semiconductor property.
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.
We present the magnetic properties of complete solid solutions of ZnCr$_2$O$_4$ and CoCr$_2$O$_4$: two well-studied oxide spinels with very different magnetic ground states. ZnCr$_2$O$_4$, with non-magnetic $d^{10}$ cations occupying the A site and magnetic $d^3$ cations on the B site, is a highly frustrated antiferromagnet. CoCr$_2$O$_4$, with magnetic $d^7$ cations (three unpaired electrons) on the A site as well, exhibits both Neel ferrimagnetism as well as commensurate and incommensurate non-collinear magnetic order. More recently, CoCr$_2$O$_4$ has been studied extensively for its polar behavior which arises from conical magnetic ordering. Gradually introducing magnetism on the A site of ZnCr$_2$O$_4$ results in a transition from frustrated antiferromagnetism to glassy magnetism at low concentrations of Co, and eventually to ferrimagnetic and conical ground states at higher concentrations. Real-space Monte-Carlo simulations of the magnetic susceptibility suggest that the first magnetic ordering transition and features of the susceptibility across $x$ are captured by near-neighbor self- and cross-couplings between the magnetic A and B atoms. We present as a part of this study, a method for displaying the temperature dependence of magnetic susceptibility in a manner which helps distinguish between compounds possessing purely antiferromagnetic interactions from compounds where other kinds of ordering are present.
We report on the results of x-ray absorption (XAS), x-ray magnetic circular dichroism (XMCD), and photoemission experiments on {it n}-type Zn$_{1-x}$Co$_x$O ($x=0.05$) thin film, which shows ferromagnetism at room temperature. The XMCD spectra show a multiplet structure, characteristic of the Co$^{2+}$ ion tetrahedrally coordinated by oxygen, suggesting that the ferromagnetism comes from Co ions substituting the Zn site in ZnO. The magnetic field and temperature dependences of the XMCD spectra imply that the non-ferromagnetic Co ions are strongly coupled antiferromagnetically with each other.
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