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Characterization of Magnetic Components in the Diluted Magnetic Semiconductor Zn$_{1-x}$Co$_x$O by X-ray Magnetic Circular Dichroism

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 Added by Masaki Kobayashi
 Publication date 2005
  fields Physics
and research's language is English




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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.



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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.
We performed a soft x-ray magnetic circular dichroism (XMCD) study of a Zn$_{1-x}$V$_x$O thin film which showed small ferromagnetic moment. Field and temperature dependences of V 2$p$ XMCD signals indicated the coexistence of Curie-Weiss paramagnetic, antiferromagnetic, and possibly ferromagnetic V ions, quantitatively consistent with the magnetization measurements. We attribute the paramagnetic signal to V ions substituting Zn sites which are somewhat elongated along the c-axis.
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.
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.
The magnetic properties of as-grown Ga$_{1-x}$Mn$_{x}$As have been investigated by the systematic measurements of temperature and magnetic field dependent soft x-ray magnetic circular dichroism (XMCD). The {it intrinsic} XMCD intensity at high temperatures obeys the Curie-Weiss law, but residual spin magnetic moment appears already around 100 K, significantly above Curie temperature ($T_C$), suggesting that short-range ferromagnetic correlations are developed above $T_C$. The present results also suggest that antiferromagnetic interaction between the substitutional and interstitial Mn (Mn$_{int}$) ions exists and that the amount of the Mn$_{int}$ affects $T_C$.
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