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We have investigated the impact of covalent hybridization on martensiticstructure and magnetic properties of Ni50Mn5+xGa35-xCu10 shape memory alloys.We found that the lattice distortion ((c-a)/a) of L10 martensite monotonouslychanges with the substitution of Mn for Ga atoms and shows a kink behavior atGa(at.%)= 25 due to the weakened covalent effect between main-group andtransition-metal atoms. Moreover, owing to the competition between covalencehybridization and magnetic ordering of introduced Mn atoms, the molecularmagnetic moment and Curie temperature coincidently show maximums at Ga(at.%)=25as well. These behaviors are closely associated with corresponding changes ofthe strength of covalent hybridization. The results therefore suggest thatcareful control of the concentration of main-group atoms in Heusler alloys canserve as an additional general tuning parameter for searching newmultifunctional materials.

Role of covalent hybridization in martensitic structure and magnetic properties of shape memory alloys: the case of Ni50Mn5+xGa35-xCu10