Structural disorder and magnetism in the spin-gapless semiconductor CoFeCrAl

Disordered CoFeCrAl and CoFeCrSi0.5Al0.5 alloys have been investigated experimentally and by first-principle calculations. The melt-spun and annealed samples all exhibit Heusler-type superlattice peaks, but the peak intensities indicate a substantial degree of B2-type chemical disorder. Si substitution reduces the degree of this disorder. Our theoretical analysis also considers several types of antisite disorder (Fe-Co, Fe-Cr, Co-Cr) in Y-ordered CoFeCrAl and partial substitution of Si for Al. The substitution transforms the spin-gapless semiconductor CoFeCrAl into a half-metallic ferrimagnet and increases the half-metallic band gap by 0.12 eV. Compared CoFeCrAl, the moment of CoFeCrSi0.5Al0.5 is predicted to increase from 2.01 μB to 2.50 μB per formula unit, in good agreement with experiment.