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Register a new userIndication of antiferromagnetic interaction between paramagnetic Co ions in the diluted magnetic semiconductor Zn$_{1-x}$Co$_{x}$O
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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.
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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.
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.
We have performed x-ray magnetic circular dichroism (XMCD) and valence-band photoemission studies of the diluted ferromagnetic semiconductor Zn$_{1-x}$Cr$_x$Te. XMCD signals due to ferromagnetism were observed at the Cr 2p absorption edge. Comparison with atomic multiplet calculations suggests that the magnetically active component of the Cr ion was divalent under the tetrahedral crystal field with tetragonal distortion along the crystalline a-, b-, and c-axes. In the valence-band spectra, spectral weight near the Fermi level was strongly suppressed, suggesting the importance of Jahn-Teller effect and the strong Coulomb interaction between the Cr 3d electrons.
The electronic structure of the Cr ions in the diluted ferromagnetic semiconductor Zn$_{1-x}$Cr$_x$Te ($x=0.03$ and 0.15) thin films has been investigated using x-ray magnetic circular dichroism (XMCD) and photoemission spectroscopy (PES). Magnetic-field ($H$) and temperature ($T$) dependences of the Cr $2p$ XMCD spectra well correspond to the magnetization measured by a SQUID magnetometer. The line shape of the Cr $2p$ XMCD spectra is independent of $H$, $T$, and $x$, indicating that the ferromagnetism is originated from the same electronic states of the Cr ion. Cluster-model analysis indicates that although there are two or more kinds of Cr ions in the Zn$_{1-x}$Cr$_x$Te samples, the ferromagnetic XMCD signal is originated from Cr ions substituted for the Zn site. The Cr 3d partial density of states extracted using Cr $2p to 3d$ resonant PES shows a broad feature near the top of the valence band, suggesting strong $s$,$p$-$d$ hybridization. No density of states is detected at the Fermi level, consistent with their insulating behavior. Based on these findings, we conclude that double exchange mechanism cannot explain the ferromagnetism in Zn$_{1-x}$Cr$_{x}$Te.
Diluted ferromagnetic semiconductors (DMSs) that combine the properties of semiconductors with ferromagnetism have potential application in spin-sensitive electronics (spintronics) devices. The search for DMS materials exploded after the observation of ferromagnetic ordering in III-V (Ga,Mn)As films. Recently, a series of DMS compounds isostructural to iron-based superconductors have been reported. Among them, the highest Curie temperature $T_C$ of 230 K has been achieved in (Ba,K)(Zn,Mn)$_2$As$_2$. However, most DMSs, including (Ga,Mn)As, are p-type, i.e., the carriers that mediate ferromagnetism are holes. For practical applications, DMS with n-type carriers are also advantageous. Here we report the successful synthesis of a II-II-V diluted ferromagnetic semiconductor with n-type carriers, Ba(Zn,Co)$_2$As$_2$. Magnetization measurements show that the ferromagnetic transition occurs up to $T_{C} sim$ 45 K. Hall effect and Seebeck effect measurements jointly confirm that the dominant carriers are electrons. Through muon spin relaxation ($mu$SR), a volume sensitive magnetic probe, we have also confirmed that the ferromagnetism in Ba(Zn,Co)$_2$As$_2$ is intrinsic and the internal field is static.
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