If magnetic semiconductors are ever to find wide application in real
spintronic devices, their magnetic and electronic properties will require
tailoring in much the same way that band gaps are engineered in conventional
semiconductors. Unfortunately, no systematic understanding yet exists of how,
or even whether, properties such as Curie temperatures and band gaps are
related in magnetic semiconductors. Here we explore theoretically these and
other relationships within 64 members of a single materials class, the Mn-doped
II-IV-V2 chalcopyrites, three of which are already known experimentally to be
ferromagnetic semiconductors. Our first-principles results reveal a variation
of magnetic properties across different materials that cannot be explained by
either of the two dominant models of ferromagnetism in semiconductors. Based on
our results for structural, electronic, and magnetic properties, we identify a
small number of new stable chalcopyrites with excellent prospects for
ferromagnetism.Comment: 6 pages with 4 figures, plus 3 supplementary figures; to appear in
Nature Material