Complex formation and background impurity of Oxygen in the PbTe:Eu doped crystals grown from melt by the Bridgman method

The magnetic field dependence of magnetization M(B) at the temperature 1.72 K in magnetic fields up to 5 T and the temperature dependence of magnetic susceptibility (M_S) χ(T) in the temperature range 1.7–400 K of six PbTe:Eu samples with the concentration of Eu impurity of the order of 1×10¹⁹–1×10²⁰ cm^?3, prepared from the doped crystals grown from the melt by the Bridgman method, have been investigated. It is shown that the dependence of M(B) and χ(T) can be quantitatively explained by the contribution of the single centers of Eu ions, their pairs, and the matrix of the doped crystals using the same set of parameters for each sample. This is true provided we use in our analysis the values of the exchange integrals between Eu ions in EuO normalized with the lattice constant of PbTe, i.e., J₁/k_B=0.056 K for the ferromagnetic interaction of the NN (nearest neighbor) pairs and J₂/k_B=?0.13 K for the antiferromagnetic interaction of the NNN (next nearest neighbor) pairs, as well as different values of the M_S of crystal χ_matrix. It is revealed that the probability of the formation of complexes based on the magnetic impurity pairs is higher in the incipient section of a doped ingot, and it decreases towards the ingot end where the single centers of Eu ions become the only centers of the impurity. We conclude that the pairs of Eu²⁺ ions, which are formed during the growth of the PbTe:Eu ingots from melt by the Bridgman method, are the constituents of the complexes of the magnetic impurities with the background Oxygen impurities in the crystal matrix of the doped lead telluride. It is shown that the formation of the complexes leads to an increase of the M_S of crystal matrix χ_matrix and can even cause the change of its sign from minus to plus, i.e., it can convert the crystal matrix from the diamagnetic to paramagnetic state. The possible causes of this effect are analyzed.