Near stoichiometric Co2FeSn Heusler alloy films with a highly ordered L2
1 structure and mean grain size of 23 ± 1 nm have been prepared on a polycrystalline copper substrate for the first time by an electrodeposition route. Deposition potential -4.0 V yielded the stoichiometric alloy composition in the potentiostatic mode. The highly disordered as-deposited alloy film crystallized into the ordered stable Heusler alloy structure upon heat treatment under vacuum. The heat-treated film exhibited the highest magnetic moment (5.18 ± 0.04 μB/f.u. at 5 K) and Curie temperature (1123 K) ever achieved in this alloy in any form. The very high value of Keff
(~106 erg/cc) obtained for this alloy makes this alloy promising for high-density magnetic recording application. Ab initio studies using GGA+U approach provide information on the minority gap near the Fermi level and its tunability as a function of the electron correlation factor represented by Hubbard parameter U.
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