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Register a new userDevelopment of magnetism in Fe-doped magnetic semiconductors: Resonant photoemission and x-ray magnetic circular dichroism studies of (Ga,Fe)As
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Fe-doped III-V ferromagnetic semiconductors (FMSs) such as (In,Fe)As, (Ga,Fe)Sb, (In,Fe)Sb, and (Al,Fe)Sb are promising materials for spintronic device applications because of the availability of both n- and p-type materials and the high Curie temperatures. On the other hand, (Ga,Fe)As, which has the same zinc-blende crystal structure as the Fe-doped III-V FMSs, shows paramagnetism. The origin of the different magnetic properties in the Fe-doped III-V semiconductors remains to be elucidated. To address this issue, we use resonant photoemission spectroscopy (RPES) and x-ray magnetic circular dichroism (XMCD) to investigate the electronic and magnetic properties of the Fe ions in a paramagnetic (Ga$_{0.95}$,Fe$_{0.05}$)As thin film. The observed Fe 2$p$-3$d$ RPES spectra show that the Fe 3$d$ states are similar to those of ferromagnetic (Ga,Fe)Sb. The estimated Fermi level is located in the middle of the band gap in (Ga,Fe)As. The Fe $L_{2,3}$ XMCD spectra of (Ga$_{0.95}$,Fe$_{0.05}$)As show pre-edge structures, which are not observed in the Fe-doped FMSs, indicating that the minority-spin ($downarrow$) $e_downarrow$ states are vacant in (Ga$_{0.95}$,Fe$_{0.05}$)As. The XMCD results suggest that the carrier-induced ferromagnetic interaction in (Ga$_{0.95}$,Fe$_{0.05}$)As is short-ranged and weaker than that in the Fe-doped FMSs. The experimental findings suggest that the electron occupancy of the $e_downarrow$ states contributes to the appearance of ferromagnetism in the Fe-doped III-V semiconductors, for p-type as well as n-type compounds.
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The question of the correlation between magnetization, band splittings, and magnetic circular dichroism (MCD) in the fundamental gap region of dilute magnetic semiconductors is examined experimentally and theoretically taking the case of wurtzite Ga(1-x)FexN as an example. Magnetization and polarization-resolved reflectivity measurements have been performed down to 2K and up to 7T for x = 0.2%. Optical transitions originating from all three free excitons A, B and C, specific to the wurtzite structure, have been observed and their evolution with the magnetic field determined. It is demonstrated that the magnitude of the exciton splittings evaluated from reflectivity-MCD data can be overestimated by more than a factor of 2, as compared to the values obtained by describing the polarization-resolved reflectivity spectra with appropriate dielectric functions. A series of model calculations shows that the quantitative inaccuracy of MCD originates from a substantial influence of the magnetization-dependent exchange interactions not only on the spin splittings of excitons but also upon their linewidth and oscillator strength. At the same time, a method is proposed that allows to evaluate the field and temperature dependencies of the magnetization from MCD spectra. The accurate values of the excitonic splittings and of the magnetization reported here substantiate the magnitudes of the apparent $sp-d$ exchange integrals in (Ga,Fe)N previously determined.
The electronic structure and the magnetism of the novel ferromagnetic semiconductor (Ga,Fe)Sb, whose Curie temperature $T_{rm C}$ can exceed room temperature, were investigated by means of x-ray absorption spectroscopy (XAS), x-ray magnetic circular dichroism (XMCD), and resonance photoemission spectroscopy (RPES). The line-shape analyses of the XAS and XMCD spectra suggest that the ferromagnetism is of intrinsic origin. The orbital magnetic moments deduced using XMCD sum rules were found to be large, indicating that there is a considerable amount of 3$d^{6}$ contribution to the ground state of Fe. From RPES, we observed a strong dispersive Auger peak and non-dispersive resonantly enhanced peaks in the valence-band spectra. The latter is a fingerprint of the correlated nature of Fe 3$d$ electrons, whereas the former indicates their itinerant nature. It was also found that the Fe 3$d$ states have finite contribution to the DOS at the Fermi energy. These states presumably consisting of majority-spin $p$-$d$ hybridized states or minority-spin $e$ states would be responsible for the ferromagnetic order in this material.
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 $T_C$.
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.
The strong perpendicular magnetic anisotropy of $L{rm1_0}$-ordered FePt has been the subject of extensive studies for a long time. However, it is not known which element, Fe or Pt, mainly contributes to the magnetic anisotropy energy (MAE). We have investigated the anisotropy of the orbital magnetic moments of Fe 3$d$ and Pt 5$d$ electrons in $L{rm1_0}$-ordered FePt thin films by Fe and Pt $L_{2,3}$-edge x-ray magnetic circular dichroism (XMCD) measurements for samples with various degrees of long-range chemical order $S$. Fe $L_{2,3}$-edge XMCD showed that the orbital magnetic moment was larger when the magnetic field was applied perpendicular to the film than parallel to it, and that the anisotropy of the orbital magnetic moment increased with $S$. Pt $L_{2,3}$-edge XMCD also showed that the orbital magnetic moment was smaller when the magnetic field was applied perpendicular to the film than parallel to it, opposite to the Fe $L_{2,3}$-edge XMCD results although the anisotropy of the orbital magnetic moment increases with $S$ like the Fe edge. These results are qualitatively consistent with the first-principles calculation by Solovyev ${it et al.}$ [Phys. Rev. B $bf{52}$, 13419 (1995).], which also predicts the dominant contributions of Pt 5$d$ to the magnetic anisotropy energy rather than Fe 3$d$ due to the strong spin-orbit coupling and the small spin splitting of the Pt 5$d$ bands in $L{rm1_0}$-ordered FePt.
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