Fully epitaxial Co 2 MnSi ͑CMS͒/MgO/CMS magnetic tunnel junctions ͑MTJs͒ with various values of Mn composition ␣ in Co 2 Mn ␣ Si electrodes were fabricated and the influence of ␣ on the tunnel magnetoresistance ͑TMR͒ characteristics of these MTJs was investigated. MTJs with Mn-rich CMS electrodes showed TMR ratios, up to 1135% at 4.2 K and 236% at room temperature for ␣ = 1.29, exceeding those of MTJs with CMS electrodes having an almost stoichiometric composition. A possible origin of the higher TMR ratios for ␣ beyond 1.0 is a decreased density of gap states existing around the Fermi level in the half-metal gap caused by the suppression of Co Mn antisites, where a Mn site is replaced by a Co atom, for Mn-rich CMS electrodes. © 2009 American Institute of Physics. ͓doi:10.1063/1.3272926͔A highly efficient spin-polarized electron source is a key element for spintronic devices. Half-metallic ferromagnets ͑HMFs͒ are the most suitable materials for spin-polarized electron sources because they provide complete spin polarization at the Fermi level ͑E F ͒. Among HMFs, Co-based Heusler alloys are especially promising due to their high Curie temperatures, which are well above room temperature ͑RT͒. Recently, extensive studies have been conducted to apply these Co-based Heusler alloy thin films to spintronic devices. [1][2][3][4][5][6][7][8] One Co-based Heusler alloy in particular, Co 2 MnSi ͑CMS͒, has attracted interest 2,4,5,7 because of its theoretically predicted half-metallic nature with a relatively large energy gap of 0.4-0.8 eV for its minority-spin direction. 9,10 We recently developed fully epitaxial magnetic tunnel junctions ͑MTJs͒ with CMS thin films as both lower and upper electrodes and with a MgO tunnel barrier ͑CMS/MgO/CMS MTJs, hereafter CMS-MTJs͒. [11][12][13] Epitaxial layer structures with a CMS electrode and a MgO barrier are beneficial for creating highly spin-polarized current due to the potentially half-metallic nature of CMS electrodes and the coherent tunneling through the single-crystalline MgO barrier. [14][15][16] We have demonstrated relatively high tunnel magnetoresistance ͑TMR͒ ratios around 180% at RT and 700% at 4.2 K for CMS-MTJs. 11,13 Furthermore, we found strong evidence for the existence of interface states in the interfacial region of CMS electrodes facing a MgO tunnel barrier, as well as evidence of residual states in the bulk region of upper CMS electrodes, in both cases in the half-metal gap for minority spins around E F from analysis of the dI / dV and d 2 I / dV 2 characteristics of CMS-MTJs. 12,13 The film composition of CMS electrodes used in our previous study [11][12][13] was Co 2 Mn 0.91 Si 0.93 , a slightly Co-rich composition with respect to the stoichiometry ͑or a slightly Mn-and Si-deficient composition͒. Film composition deviation from the stoichiometry inevitably induces some kinds of structural defect. The influence of defects in CMS on the half-metallic electronic structure has been investigated theoretically. [17][18][19][20] It has been pointed out that the half...