Magnetooptical properties of (Ga,Mn)N layers containing various concentrations of Fe-rich nanocrystals embedded in paramagnetic (Ga,Fe)N layers are reported. Previous studies of such samples demonstrated that magnetization consists of a paramagnetic
contribution due to substitutional diluted Fe ions as well as of ferromagnetic and antiferromagnetic components originating from Fe-rich nanocrystals, whose relative abundance can be controlled by the grow conditions. The nanocrystals are found to broaden and to reduce the magnitude of the excitonic features. However, the ferromagnetic contribution, clearly seen in SQUID magnetometry, is not revealed by magnetic circular dichroism (MCD). Possible reasons for differences in magnetic response determined by MCD and SQUID measurements are discussed.
The question of the correlation between magnetization, band splittings, and magnetic circular dichroism (MCD) in the fundamental gap region of dilute magnetic semiconductors is examined experimentally and theoretically taking the case of wurtzite Ga(
1-x)FexN as an example. Magnetization and polarization-resolved reflectivity measurements have been performed down to 2K and up to 7T for x = 0.2%. Optical transitions originating from all three free excitons A, B and C, specific to the wurtzite structure, have been observed and their evolution with the magnetic field determined. It is demonstrated that the magnitude of the exciton splittings evaluated from reflectivity-MCD data can be overestimated by more than a factor of 2, as compared to the values obtained by describing the polarization-resolved reflectivity spectra with appropriate dielectric functions. A series of model calculations shows that the quantitative inaccuracy of MCD originates from a substantial influence of the magnetization-dependent exchange interactions not only on the spin splittings of excitons but also upon their linewidth and oscillator strength. At the same time, a method is proposed that allows to evaluate the field and temperature dependencies of the magnetization from MCD spectra. The accurate values of the excitonic splittings and of the magnetization reported here substantiate the magnitudes of the apparent $sp-d$ exchange integrals in (Ga,Fe)N previously determined.
This work presents results of near-band gap magnetooptical studies on (Zn,Mn)O epitaxial layers. We observe excitonic transitions in reflectivity and photoluminescence, that shift towards higher energies when the Mn concentration increases and split
nonlinearly under the magnetic field. Excitonic shifts are determined by the s,p-d exchange coupling to magnetic ions, by the electron-hole s-p exchange, and the spin-orbit interactions. A quantitative description of the magnetoreflectivity findings indicates that the free excitons A and B are associated with the Gamma_7 and Gamma_9 valence bands, respectively, the order reversed as compared to wurtzite GaN. Furthermore, our results show that the magnitude of the giant exciton splittings, specific to dilute magnetic semiconductors, is unusual: the magnetoreflectivity data is described by an effective exchange energy N_0(beta-alpha)=+0.2+/-0.1 eV, what points to small and positive N_0 beta. It is shown that both the increase of the gap with x and the small positive value of the exchange energy N_0 beta corroborate recent theory describing the exchange splitting of the valence band in a non-perturbative way, suitable for the case of a strong p-d hybridization.
A direct observation of the giant Zeeman splitting of the free excitons in (Ga,Fe)N is reported. The magnetooptical and magnetization data imply the ferromagnetic sign and a reduced magnitude of the effective p-d exchange energy governing the interac
tion between Fe^{3+} ions and holes in GaN, N_0 beta^(app) = +0.5 +/- 0.2 eV. This finding corroborates the recent suggestion that the strong p-d hybridization specific to nitrides and oxides leads to significant renormalization of the valence band exchange splitting.
