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The effects of Gd doping and O vacancies on the magnetic interaction andCurie temperature of EuO are studied using first-principles calculations.Linear response calculations in the virtual crystal approximation show a broadmaximum in the Curie temperature as a function of doping, which results fromthe combination of the saturating contribution from indirect exchange and adecreasing contribution from the f-d hopping mechanism. Non-Heisenberginteraction at low doping levels and its effect on the Curie temperature areexamined. The electronic structure of a substitutional Gd and of an O vacancyin EuO are evaluated. When the 4f spins are disordered, the impurity state goesfrom single to double occupation, but correlated bound magnetic polarons arenot ruled out. At higher vacancy concentrations typical for Eu-rich EuO films,the impurity states broaden into bands and remain partially filled. To gobeyond the homogeneous doping picture, magnetostructural cluster expansions areconstructed, which describe the modified exchange parameters near Gd dopants orO vacancies. Thermodynamic properties are studied using Monte Carlosimulations. The Curie temperature for Gd-doped EuO agrees with the results ofthe virtual crystal approximation and shows a maximum of about 150 K. At 3.125%vacancy concentration the Curie temperature increases to 120 K, consistent withexperimental data for Eu-rich film samples.

Electronic structure and magnetic properties of Gd-doped and Eu-rich EuO