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Register a new userMinority-Spin Impurity Band in n-Type (In,Fe)As: A Materials Perspective for Ferromagnetic Semiconductors
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Fully understanding the properties of n-type ferromagnetic semiconductors (FMSs), complementary to the mainstream p-type ones, is a challenging goal in semiconductor spintronics because ferromagnetism in n-type FMSs is theoretically non-trivial. Soft-x-ray angle-resolved photoemission spectroscopy (SX-ARPES) is a powerful approach to examine the mechanism of carrier-induced ferromagnetism in FMSs. Here our SX-ARPES study on the prototypical n-type FMS (In,Fe)As reveals the entire band structure including the Fe-3d impurity bands (IBs) and the host InAs ones, and provides direct evidence for electron occupation of the InAs-derived conduction band (CB). A minority-spin Fe-3d IB is found to be located just below the conduction-band minimum (CBM). The IB is formed by the hybridization of the unoccupied Fe-3d states with the occupied CBM of InAs in a spin-dependent way, resulting in the large spin polarization of CB. The band structure with the IB is varied with band filling, which cannot be explained by the rigid-band picture, suggesting a unified picture for realization of carrier-induced ferromagnetism in FMS materials.
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The electronic and magnetic properties of Fe atoms in the ferromagnetic semiconductor (In,Fe)As codoped with Be have been studied by x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) at the Fe $L_{2,3}$ edge. The XAS and XMCD spectra showed simple spectral line shapes similar to Fe metal, but the ratio of the orbital and spin magnetic moments ($M_mathrm{orb}$/$M_mathrm{spin}$) estimated using the XMCD sum rules was significantly larger than that of Fe metal, indicating a significant orbital moment of Fe $3d$ electrons in (In,Fe)As:Be. The positive value of $M_mathrm{orb}$/$M_mathrm{spin}$ implies that the Fe $3d$ shell is more than half-filled, which arises from the hybridization of the Fe$^{3+}$ ($d^5$) state with the charge-transfer $d^6underline{L}$ states, where $underline{L}$ is a ligand hole in the host valence band. The XMCD intensity as a function of magnetic field indicated hysteretic behavior of the superparamagnetic-like component due to discrete ferromagnetic domains.
(Ga$_{1-x}$,Fe$_x$)Sb is one of the promising ferromagnetic semiconductors for spintronic device applications because its Curie temperature ($T_{rm C}$) is above 300 K when the Fe concentration $x$ is equal to or higher than ~0.20. However, the origin of the high $T_{rm C}$ in (Ga,Fe)Sb remains to be elucidated. To address this issue, we use resonant photoemission spectroscopy (RPES) and first-principles calculations to investigate the $x$ dependence of the Fe 3$d$ states in (Ga$_{1-x}$,Fe$_x$)Sb ($x$ = 0.05, 0.15, and 0.25) thin films. The observed Fe 2$p$-3$d$ RPES spectra reveal that the Fe-3$d$ impurity band (IB) crossing the Fermi level becomes broader with increasing $x$, which is qualitatively consistent with the picture of double-exchange interaction. Comparison between the obtained Fe-3$d$ partial density of states and the first-principles calculations suggests that the Fe-3$d$ IB originates from the minority-spin ($downarrow$) $e$ states. The results indicate that enhancement of the interaction between $e_downarrow$ electrons with increasing $x$ is the origin of the high $T_{rm C}$ in (Ga,Fe)Sb.
We show that by introducing isoelectronic iron (Fe) magnetic impurities and Beryllium (Be) double-donor atoms into InAs, it is possible to grow a n-type ferromagnetic semiconductor (FMS) with the ability to control ferromagnetism by both Fe and independent carrier doping by low-temperature molecular-beam epitaxy. We demonstrate that (In,Fe)As doped with electrons behaves as an n-type electron-induced FMS. This achievement opens the way to realize novel spin-devices such as spin light-emitting diodes or spin field-effect transistors, as well as helps understand the mechanism of carrier-mediated ferromagnetism in FMSs.
The element-specific technique of x-ray magnetic circular dichroism (XMCD) is used to directly determine the magnitude and character of the valence band orbital magnetic moments in (III,Mn)As ferromagnetic semiconductors. A distinct dichroism is observed at the As K absorption edge, yielding an As 4p orbital magnetic moment of around -0.1 Bohr magnetons per valence band hole. This is strongly influenced by strain, indicating its crucial influence on the magnetic anisotropy. The dichroism at the Ga K edge is much weaker. The K edge XMCD signals for Mn and As both have positive sign, which indicates the important contribution of Mn 4p states to the Mn K edge spectra.
We present high-temperature ferromagnetism and large magnetic anisotropy in heavily Fe-doped n-type ferromagnetic semiconductor (In1-x,Fex)Sb (x = 20 - 35%) thin films grown by low-temperature molecular beam epitaxy. The (In1-x,Fex)Sb thin films with x = 20 - 35% maintain the zinc-blende crystal and band structure with single-phase ferromagnetism. The Curie temperature (TC) of (In1-x,Fex)Sb reaches 390 K at x = 35%, which is significantly higher than room temperature and the highest value so far reported in III-V based ferromagnetic semiconductors. Moreover, large coercive force (HC = 160 Oe) and large remanent magnetization (Mr/MS = 71%) have been observed for a (In1-x,Fex)Sb thin film with x = 35%. Our results indicate that the n-type ferromagnetic semiconductor (In1-x,Fex)Sb is very promising for spintronics devices operating at room temperature.
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