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Register a new userFerromagnetism in ZnO co-doped with Mn and N studied by soft x-ray magnetic circular dichroism
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We have investigated the electronic structure of ZnO:Mn and ZnO:Mn,N thin films using x-ray magnetic circular dichroism (XMCD) and resonance-photoemission spectroscopy. From the Mn 2$p$$rightarrow3d$ XMCD results, it is shown that, while XMCD signals only due to paramagnetic Mn$^{2+}$ ions were observed in ZnO:Mn, nonmagnetic, paramagnetic and ferromagnetic Mn$^{2+}$ ions coexist in ZnO:Mn,N. XMCD signals of ZnO:Mn,N revealed that the localized Mn$^{2+}$ ground state and Mn$^{2+}$ state hybridized with ligand hole coexisted, implying $p$-$d$ exchange coupling. In the valence-band spectra, spectral weight near the Fermi level was suppressed, suggesting that interaction between magnetic moments in ZnO:Mn,N has localized nature.
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We report on x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) studies of the paramagnetic (Mn,Co)-co-doped ZnO and ferromagnetic (Fe,Co)-co-doped ZnO nano-particles. Both the surface-sensitive total-electron-yield mode and the bulk-sensitive total-fluorescence-yield mode have been employed to extract the valence and spin states of the surface and inner core regions of the nano-particles. XAS spectra reveal that significant part of the doped Mn and Co atoms are found in the trivalent and tetravalent state in particular in the surface region while majority of Fe atoms are found in the trivalent state both in the inner core region and surface region. The XMCD spectra show that the Fe$^{3+}$ ions in the surface region give rise to the ferromagnetism while both the Co and Mn ions in the surface region show only paramagnetic behaviors. The transition-metal atoms in the inner core region do not show magnetic signals, meaning that they are antiferromagnetically coupled. The present result combined with the previous results on transition-metal-doped ZnO nano-particles and nano-wires suggest that doped holes, probably due to Zn vacancy formation at the surfaces of the nano-particles and nano-wires, rather than doped electrons are involved in the occurrence of ferromagnetism in these systems.
BiFeO$_3$ (BFO) shows both ferroelectricity and magnetic ordering at room temperature but its ferromagnetic component, which is due to spin canting, is negligible. Substitution of transition-metal atoms such as Co for Fe is known to enhance the ferromagnetic component in BFO. In order to reveal the origin of such magnetization enhancement, we performed soft x-ray absorption spectroscopy (XAS) and soft x-ray magnetic circular dichroism (XMCD) studies of BiFe$_{1-x}$Co$_x$O$_3$ ({it x} = 0 to 0.30) (BFCO) thin films grown on LaAlO$_3$(001) substrates. The XAS results indicated that the Fe and Co ions are in the Fe$^{3+}$ and Co$^{3+}$ states. The XMCD results showed that the Fe ions show ferromagnetism while the Co ions are antiferromagnetic at room temperature. The XAS and XMCD measurements also revealed that part of the Fe$^{3+}$ ions are tetrahedrally co-ordinated by oxygen ions but that the XMCD signals of the octahedrally coordinated Fe$^{3+}$ ions increase with Co content. The results suggest that an impurity phase such as the ferrimagnetic $gamma$-Fe$_2$O$_3$ which exists at low Co concentration decreases with increasing Co concentration and that the ferromagnetic component of the Fe$^{3+}$ ion in the octrahedral crystal fields increases with Co concentration, probably reflecting the increased canting of the Fe$^{3+}$ ions.
We have studied magnetism in anatase Ti$_{1-x}$Co$_x$O$_{2-delta}$ ({it x} = 0.05) thin films with various electron carrier densities, by soft x-ray magnetic circular dichroism (XMCD) measurements at the Co $L_{2,3}$ absorption edges. For electrically conducting samples, the magnetic moment estimated by XMCD was $<$ 0.3 $mu_B$/Co using the surface-sensitive total electron yield (TEY) mode, while it was 0.3-2.4 $mu_B$/Co using the bulk-sensitive total fluorescence yield (TFY) mode. The latter value is in the same range as the saturation magnetization 0.6-2.1 $mu_B$/Co deduced by SQUID measurement. The magnetization and the XMCD intensity increased with carrier density, consistent with the carrier-induced origin of the ferromagnetism.
We have studied the electronic structure of the molecular ferromagnet $beta$-Mn phthalocyanine ($beta$-MnPc) in a polycrystalline form, which has been reported to show ferromagnetism at T$<$8.6 K, by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD). From the experimental results and subsequent cluster-model calculation, we find that the ferromagnetic Mn ion in $beta$-MnPc is largely in the $^4$$E$$_g$ ground state arising from the ($e$$_{g}$)$^3$($b$$_{2g}$)$^1$($a$$_{1g}$)$^1$ [($d_{xz,yz}$)$^3$($d_{xy}$)$^1$($d_{z^{2}}$)$^1$] configuration of the Mn$^{2+}$ state. Considering that the highest occupied molecular orbital (HOMO) of MnPc with the $^4$$E$$_g$ ground state originates from the $a$$_{1g}$ orbital of the Mn$^{2+}$ ion, it is proposed that $a$$_{1g}$-$a$$_{1g}$ exchange coupling via the $pi$ orbitals of the phthalocyanine ring plays a crucial role in the ferromagnetism of $beta$-MnPc.
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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