Microcrystalline Ga1−xMnxN samples with Mn content up to x=0.005 were grown by an ammonothermal method and were studied using various techniques. X-ray diffraction showed characteristic diffraction lines for hexagonal GaN phase mixed with a small contribution (<5%) from the Mn3N2 phase. Raman spectra exhibited characteristic peaks of pure GaN and modes that could be associated with Mn-induced lattice disorder. Electron spin resonance and magnetization measurements were consistent with the dominant Mn2+(d5) configuration of spin S=5/2 which is responsible for the observed paramagnetic behavior of the GaMnN material.
Magnetic circular dichroism (MCD) of a ferromagnetic diluted magnetic semiconductor films was measured to clarify their electronic structure. Strong enhancement of MCD by Mn substitution indicated a strong hybridization. The exchange interaction was concluded to be antiferromagnetic, which was in contrast with the reported ferromagnetic exchange in very diluted paramagnetic GaAs:Mn bulk crystals. The change of the character of the exchange interaction is due to the unique feature of that the relative abundance of the neutral and ionized Mn acceptors controls the exchange.
The exchange interaction of p-type epilayers is investigated by means of magnetoabsorption. The observed ferromagnetic-type splitting of fundamental absorption edge is explained by antiferromagnetic exchange interaction, taking into account the Moss-Burstein effect, resulting from high hole concentration.
The magnetization of Ga1−xMnxN (x<0.1) crystals was measured as a function of the magnetic field and temperature. Paramagnetic behavior typical of spin S=5/2 expected for Mn2+ (d5) magnetic centers was observed in the temperature range of 2 K<T<300 K. On the other hand, antiferromagnetic coupling between Mn ions was clearly visible. The nearest neighbor (NN) coupling constant JNN/kB=−1.9 K was estimated from the temperature dependence of the magnetization.
The magnetic susceptibility and specific heat of the diluted magnetic semiconductor Se have been measured in the temperature range 10 mK<T<40 K for 0.01≤x≤0.53. A paramagnetic–spin-glass transition was observed in the whole concentration range. The concentration dependence of the freezing temperature was found to be compatible with a radial dependence of the exchange interaction between manganese ions of the type J(R)∼. Based on this observation, we calculated thermodynamic properties with the extended nearest-neighbor pair approximation. It appears that this approximation provides a good simultaneous description of the specific heat and high-field magnetization and reproduces Curie-Weiss temperature for parameters /=-13 K (nearest-neighbor interaction) and (R)/=-7/ K (distant-neighbor interaction). A comparison is made with other dilute magnetic semiconductors, and the possible origin of the exchange mechanism is then discussed.