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Register a new userMicroscopic analysis of the valence band and impurity band theories of (Ga,Mn)As
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We analyze microscopically the valence and impurity band models of ferromagnetic (Ga,Mn)As. We find that the tight-binding Anderson approach with conventional parameterization and the full potential LDA+U calculations give a very similar picture of states near the Fermi energy which reside in an exchange-split sp-d hybridized valence band with dominant orbital character of the host semiconductor; this microscopic spectral character is consistent with the physical premise of the k.p kinetic-exchange model. On the other hand, the various models with a band structure comprising an impurity band detached from the valence band assume mutually incompatible microscopic spectral character. By adapting the tight-binding Anderson calculations individually to each of the impurity band pictures in the single Mn impurity limit and then by exploring the entire doping range we find that a detached impurity band does not persist in any of these models in ferromagnetic (Ga,Mn)As.
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We discuss the character of states near the Fermi level in Mn doped GaAs, as revealed by a survey of dc transport and optical studies over a wide range of Mn concentrations. A thermally activated valence band contribution to dc transport, a mid-infrared peak at energy hbar omega approx 200 meV in the ac- conductivity, and the hot photoluminescence spectra indicate the presence of an impurity band in low doped (<<1% Mn) insulating GaAs:Mn materials. Consistent with the implications of this picture, both the impurity band ionization energy inferred from the dc transport and the position of the mid-infrared peak move to lower energies and the peak broadens with increasing Mn concentration. In metallic materials with > 2% doping, no traces of Mn-related activated contribution can be identified in dc-transport, suggesting that the impurity band has merged with the valence band. No discrepancies with this perception are found when analyzing optical measurements in the high-doped GaAs:Mn. A higher energy (hbar omega approx 250 meV) mid-infrared feature which appears in the metallic samples is associated with inter-valence band transitions. Its red-shift with increased doping can be interpreted as a consequence of increased screening which narrows the localized-state valence-band tails and weakens higher energy transition amplitudes. Our examination of the dc and ac transport characteristics of GaAs:Mn is accompanied by comparisons with its shallow acceptor counterparts, confirming the disordered valence band picture of high-doped metallic GaAs:Mn material.
(Ga,Mn)As is a paradigm diluted magnetic semiconductor which shows ferromagnetism induced by doped hole carriers. With a few controversial models emerged from numerous experimental and theoretical studies, the mechanism of the ferromagnetism in (Ga,Mn)As still remains a puzzling enigma. In this Letter, we use soft x-ray angle-resolved photoemission spectroscopy to positively identify the ferromagnetic Mn 3d-derived impurity band in (Ga,Mn)As. The band appears hybridized with the light-hole band of the host GaAs. These findings conclude the picture of the valence band structure of (Ga,Mn)As disputed for more than a decade. The non-dispersive character of the IB and its location in vicinity of the valence-band maximum indicate that the Mn 3d-derived impurity band is formed as a split-off Mn-impurity state predicted by the Anderson impurity model. Responsible for the ferromagnetism in (Ga,Mn)As is the transport of hole carriers in the impurity band.
We report high-resolution hard x-ray photoemission spectroscopy results on (Ga,Mn)As films as a function of Mn doping. Supported by theoretical calculations we identify, over the entire 1% to 13% Mn doping range, the electronic character of the states near the top of the valence band. Magnetization and temperature dependent core-level photoemission spectra reveal how the delocalized character of the Mn states enables the bulk ferromagnetic properties of (Ga,Mn)As.
Modulation photoreflectance spectroscopy and Raman spectroscopy have been applied to study the electronic- and band-structure evolution in (Ga,Mn)As epitaxial layers with increasing Mn doping in the range of low Mn content, up to 1.2%. Structural and magnetic properties of the layers were characterized with high-resolution X-ray diffractometry and SQUID magnetometery, respectively. The revealed results of decrease in the band-gap transition energy with increasing Mn content in very low-doped (Ga,Mn)As layers with n-type conductivity are interpreted as a result of merging the Mn-related impurity band with the host GaAs valence band. On the other hand, an increase in the band-gap-transition energy with increasing Mn content in (Ga,Mn)As layers with higher Mn content and p-type conductivity indicates the Moss-Burstein shift of the absorption edge due to the Fermi level location within the valence band, determined by the free-hole concentration. The experimental results are consistent with the valence-band origin of mobile holes mediated ferromagnetic ordering in the (Ga,Mn)As diluted ferromagnetic semiconductor.
The effect of outdiffusion of Mn interstitials from (Ga,Mn)As epitaxial layers, caused by post-growth low-temperature annealing, on their electronic- and band-structure properties has been investigated by modulation photoreflectance (PR) spectroscopy. The annealing-induced changes in structural and magnetic properties of the layers were examined with high-resolution X-ray diffractometry and SQUID magnetometery, respectively. They confirmed an outdiffusion of Mn interstitials from the layers and an enhancement in their hole concentration, which were more efficient for the layer covered with a Sb cap acting as a sink for diffusing Mn interstitials. The PR results revealing a decrease in the band-gap-transition energy in the as-grown (Ga,Mn)As layers, with respect to that in the reference GaAs one, are interpreted by assuming a merging of the Mn-related impurity band with the host GaAs valence band. On the other hand, an increase in the band-gap-transition energy in the annealed (Ga,Mn)As layers is interpreted as a result of the Moss-Burstein shift of the absorption edge due to the Fermi level location within the valence band, determined by the enhanced free-hole concentration. The experimental results are consistent with the valence-band origin of mobile holes mediating ferromagnetic ordering in (Ga,Mn)As, in agreement with the Zener model for ferromagnetic semiconductors.
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