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Register a new userElectronic- and band-structure evolution in low-doped (Ga,Mn)As
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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.
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The detailed nature of electronic states mediating ferromagnetic coupling in dilute magnetic semiconductors, specifically (Ga,Mn)As, has been an issue of long debate. Two confronting models have been discussed emphasizing host band vs. impurity band carriers. Using angle resolved photoemission we are for the first time able to identify a highly dispersive Mn-induced energy band in (Ga,Mn)As. Our results show that the electronic structure of the (Ga,Mn)As system is significantly modified from that of GaAs throughout the valence band. Close to the Fermi energy, the presence of Mn induces a strong mixing of the bulk bands of GaAs, which results in the appearance of a highly dispersive band in the gap region of GaAs. For Mn concentrations above 1% the band reaches the Fermi level, and can thus host the delocalized holes needed for ferromagnetic coupling. Overall, our data provide a firm evidence of delocalized carriers belonging to the modified host valence band.
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.
A remarkable progress towards functional ferromagnetic semiconductor materials for spintronics has been achieved in p-type (Ga,Mn)As. Robust hole-mediated ferromagnetism has, however, been observed also in other III-V hosts such as antimonides, GaP or (Al,Ga)As which opens a wide area of possibilities for optimizing the host composition towards higher ferromagnetic Curie temperatures. Here we explore theoretically ferromagnetism and Mn incorporation in Ga(As,P) and (Al,Ga)As ternary hosts. While alloying (Ga,Mn)As with Al has only a small effect on the Curie temperature we predict a sizable enhancement of Curie temperatures in the smaller lattice constant Ga(As,P) hosts. Mn-doped Ga(As,P) is also favorable, as compared to (Al,Ga)As, with respect to the formation of carrier and moment compensating interstitial Mn impurities. In (Ga,Mn)(As,P) we find a marked decrease of the partial concentration of these detrimental impurities with increasing P content.
We have investigated the electronic structure of the $p$-type diluted magnetic semiconductor In$_{1-x}$Mn$_x$As by photoemission spectroscopy. The Mn 3$d$ partial density of states is found to be basically similar to that of Ga$_{1-x}$Mn$_x$As. However, the impurity-band like states near the top of the valence band have not been observed by angle-resolved photoemission spectroscopy unlike Ga$_{1-x}$Mn$_x$As. This difference would explain the difference in transport, magnetic and optical properties of In$_{1-x}$Mn$_x$As and Ga$_{1-x}$Mn$_x$As. The different electronic structures are attributed to the weaker Mn 3$d$ - As 4$p$ hybridization in In$_{1-x}$Mn$_x$As than in Ga$_{1-x}$Mn$_x$As.
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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