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Register a new userResponse to the comment of K.W. Edmonds et al. on the article Controlling the Curie temperature in (Ga,Mn)As through location of the Fermi level within the impurity band
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Although we seriously disagree with many of the points raised in the comment by Edmonds et al., we feel that it is valuable and timely, since comparison of this comment and our paper serves to underscore an important property of the ferromagnetic semiconductor (Ga,Mn)As in thin film form.
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Comment on the recent Nature Materials article by M. Dobrowolska et al., arXiv:1203.1852. We present experimental data showing that the Curie temperature and conductivity of high quality (Ga,Mn)As samples are maximized at low compensation, and thus the magnetic order in (Ga,Mn)As is not consistent with the isolated impurity band scenario.
The ferromagnetic semiconductor (Ga,Mn)As has emerged as the most studied material for prototype applications in semiconductor spintronics. Because ferromagnetism in (Ga,Mn)As is hole-mediated, the nature of the hole states has direct and crucial bearing on its Curie temperature TC. It is vigorously debated, however, whether holes in (Ga,Mn)As reside in the valence band or in an impurity band. In this paper we combine results of channeling experiments, which measure the concentrations both of Mn ions and of holes relevant to the ferromagnetic order, with magnetization, transport, and magneto-optical data to address this issue. Taken together, these measurements provide strong evidence that it is the location of the Fermi level within the impurity band that determines TC through determining the degree of hole localization. This finding differs drastically from the often accepted view that TC is controlled by valence band holes, thus opening new avenues for achieving higher values of TC.
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.
We study the effects of growth temperature, Ga:As ratio and post-growth annealing procedure on the Curie temperature, Tc, of (Ga,Mn)As layers grown by molecular beam epitaxy. We achieve the highest Tc values for growth temperatures very close to the 2D-3D phase boundary. The increase in Tc, due to the removal of interstitial Mn by post growth annealing, is counteracted by a second process which reduces Tc and which is more effective at higher annealing temperatures. Our results show that it is necessary to optimize the growth parameters and post growth annealing procedure to obtain the highest Tc.
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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