Ge 1−x Fe x (Ge:Fe) shows ferromagnetic behavior up to a relatively high temperature of 210 K, and hence is a promising material for spintronic applications compatible with Si technology. We have studied its electronic structure by soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) measurements in order to elucidate the mechanism of the ferromagnetism. We observed finite Fe 3d components in the states at the Fermi level (E F ) in a wide region in momentum space and E F was located above the valenceband maximum (VBM). First-principles supercell calculation also suggested that the E F is located above the VBM, within the narrow spin-down d(e) band and within the spin-up impurity band of the deep acceptor-level origin derived from the strong p-d(t 2 ) hybridization. We conclude that the narrow d(e) band is responsible for the ferromagnetic coupling between Fe atoms while the acceptor-level-originated band is responsible for the transport properties of Ge:Fe.
1Ferromagnetic semiconductors (FMSs) such as (Ga,Mn)As [1, 2] have attracted much attention both from scientific and technological points of view [3][4][5][6][7][8]. Group-IV FMSs are particularly important because they are compatible with mature Si-based technology. Ge 1−x Fe x (Ge:Fe) is a promising material [9][10][11][12], and indeed can be grown epitaxially on Ge and Si substrates by the low-temperature molecular beam epitaxy (LT-MBE) method without the formation of intermetallic precipitates [13]. It shows p-type conduction, but the carrier concentration of ∼10 18 cm −3 [13] is orders of magnitude smaller than that of doped Fe atoms (∼10 21 cm −3 ). The Curie temperature (T C ) increases with the Fe content and with the inhomogeneity of Fe atom distribution [11,12], and reaches ∼210 K at highest by post-growth annealing [11], which is above the highest T C of (Ga,Mn)As, ∼200 K [14]. Unlike (Ga,Mn)As, the T C does not depend on carrier concentration [13]. Recent x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements [15] have revealed the valence of Fe substituting Ge to be 2+, which indicates that each Fe atoms would provide two holes. It was also found that nanoscale ferromagnetic domains exist even above the T C , the origin of which was attributed to the inhomogeneous distribution of Fe atoms on the nanoscale.In order to explain the origin of the ferromagnetism in (Ga,Mn)As and related FMSs, two models have been proposed so far [5,16,17], namely, the valence-band model [18,19] and the impurity-band model [20][21][22][23]. In the valence-band model, acceptor levels derived from the magnetic impurities are merged into the valence band and itinerant holes occupying states around the valence-band maximum (VBM) mediate ferromagnetism through Zener's p-d exchange mechanism.In the case of the impurity-band model, on the other hand, impurity levels are detached from the VBM and lies within the band gap of the host semiconductor and hence ferromagnetism is stabilized through a double-exchange-like mec...