Diluted ferromagnetic semiconductors combining ferromagnetic and semiconducting properties in one material provide numerous new functionalities, attractive for basic studies and potentially useful for novel device applications. The tailoring of the electronic structure in analogy to conventional semiconductors has yet to be explored. Here, we demonstrate the conservation of broken inversion symmetry and band structure tailoring for high-quality molecular-beam-epitaxy-grown (In,Ga,Mn)As films with 3% In plus 2.5% or 5.6% Mn using hard-x-ray photoelectron diffraction (hXPD) and momentum microscopy. Photon energies of 3-5 keV ensure that the results are not corrupted by surface effects, which are known to be strong in semiconductors. The missing inversion center of the GaAs host lattice leads to fingerprint-like hXPD signatures of As and Ga sites. For both concentrations, Mn predominantly occupies Ga substitutional sites. Momentum microscopy reveals a shift of the chemical potential with increasing Mn doping and a highly dispersing band, crossing the Fermi level for high Mn concentration. The Mn doping induces a pronounced modification of the spin-orbit split-off band.
Impact of Bi incorporation into (Ga,Mn)As layers on their electronic- and band-structures as well as their magnetic and structural properties has been studied. Homogenous (Ga,Mn)(Bi,As) layers of high structural perfection have been grown by the low-temperature molecular-beam epitaxy technique. Post-growth annealing treatment of the layers results in an improvement of their structural and magnetic properties and an increase in the hole concentration in the layers. The modulation photoreflectance spectroscopy results are consistent with the valence-band model of hole-mediated ferromagnetism in the layers. This material combines the properties of (Ga,Mn)As and Ga(Bi,As) ternary compounds and offers the possibility of tuning its electrical and magnetic properties by controlling the alloy composition.
The high-spectral-resolution spectroscopic studies of the energy gap evolution, supplemented with electronic, magnetic and structural characterization, show that the modification of the GaAs valence band caused by Mn incorporation occurs already for a very low Mn content, much lower than that required to support ferromagnetic spin -spin coupling in (Ga,Mn)As. Only for n-type (Ga,Mn)As with the Mn content below about 0.3% the Mnrelated extended states are visible as a feature detached from the valence-band edge and partly occupied with electrons. The combined magnetic and low-temperature photoreflectance studies presented here indicate that the paramagnetic -ferromagnetic transformation in p-type (Ga,Mn)As takes place without imposing changes of the unitary character of the valence band with the Fermi level located therein. The whole process is rooted in the nanoscale fluctuations of the local (hole) density of states and the formation of a superparamagnetic-like state. The Fermi level in (Ga,Mn)As is coarsened by the carrier concentration of the itinerant valence band holes and further fine-tuned by the many-body interactions.
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