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Zusammenfassung:
The tunnel magnetoresistance ratio (TMR) of fully epitaxial magnetic tunnel junctions with an off-stoichiometric Co2MnSi Heusler alloy has been shown to exhibit a systematic dependence on Mn content, reaching 1135% at 4.2 K for Co2Mn1.29Si. In this paper, we explain the behavior of the observed TMR ratio using ab initio calculations and hard x-ray photoelectron spectroscopy (HAXPES). For the Mn-deficient samples, we show that the the drop of the TMR is caused by Co antisite atoms, which impose extra states into the minority-spin band gap. On the other hand, Mn-excess composition shows nearly half-metallic behavior. This result can be intuitively understood since both Co2MnSi and Mn2CoSi are theoretically predicted to be half-metallic ferromagnets.