Spin polarization and Gilbert damping of Co2Fe(GaxGe1−x) Heusler alloys
Introduction
Half-metallic ferromagnets (HFMs) were first proposed theoretically for half-Heusler NiMnSb and PtMnSb alloys by de Groot et al. [1]. Subsequently, several Co-based full Heusler alloys with the L21 structure were also predicted to be half-metal with high Curie temperatures [2]. The interest in Heusler alloys as spin polarized electron sources was boosted with the demonstration of the huge giant tunneling magnetoresistance (TMR) ratio of 570% at 2 K in the Co2MnSi/Al–O/Co2MnSi magnetic tunneling junction (MTJ) by Sakuraba et al. [3] The high TMR value was attributed to the half-metallic nature of the Co2MnSi Heusler alloy; however, the TMR value of this MTJ is degraded at room temperature (RT) to only 67%. The reason for this large temperature degradation of TMR is considered to be due to the presence of quasi-particle states in the spin-down density of states at the Fermi level, which causes a large decrease in the spin polarization at room temperature. Fermi level tuning by alloying a fourth element to ternary Heusler alloys has been proposed to circumvent this problem and Co2Fe(Al1−xSix) was the first such material to be was investigated along these lines [4], [5], [6]. Tezuka et al. demonstrated the Fermi level tuning in Co2Fe(Al0.5Si0.5) experimentally [5], a finding that was also supported by ab initio calculations of the density of states (DOS) [4] and by our previous point contact Andreev reflection (PCAR) measurements [6], [7]. Subsequently, several theoretical calculations showed the possibility of improving the spin polarization of Heusler alloys with site disorders by Fermi level tuning [8], [9].
We have systematically sought highly spin-polarized ferromagnetic (FM) alloys by PCAR measurements [6], [7], [10], [11]. Our search has led to the finding of highly spin-polarized Co-based quaternary Heusler alloys such as Co2(Fe1−xCrx)Si [6], Co2Mn(Ga0.5Sn0.5) [10], Co2Mn(Ga0.5Ge0.5) [11] and Co2Fe(Ga0.5Ge0.5) [12]. We also applied these alloys as FM layers of current-perpendicular-to-plane giant magnetoresistive (CPP-GMR) devices and found that all of these gave rise to a rather high magnetoresistive area product change (ΔRA) of >6 mΩ μm2, which is more than three times larger than can be obtained from the CPP-GMR devices using normal FM alloys, i.e. 1–2 mΩ μm2. Among these alloys, the Co2Fe(Ga0.5Ge0.5) alloy is of particular interest because its use as FM layers led to ΔRA of 9.5 mΩ μm2 and an MR ratio exceeding 41% at room temperature [12]. The alloy composition used in the CPP-GMR device has been optimized using bulk alloys; thereafter films with an optimized composition have been prepared. In this paper, we report a systematic investigation on the structure, magnetic properties and intrinsic spin polarization of bulk Co2Fe(GaxGe1−x) alloys. The magnetic and transport properties of the films of optimized Co2Fe(Ga0.5Ge0.5) alloy were also investigated.
Section snippets
Experimental
Bulk Co2Fe(GaxGe1−x) (x = 0, 0.25, 0.5, 0.75, and 1) alloys were prepared by arc melting high-purity elements in an Ar atmosphere. The alloys were annealed in evacuated fused silica tubes for 168 h at 673 K to attain phase equilibria. Curie temperatures (Tc), L21 ↔ B2 order–disorder and melting temperatures were measured by differential thermal analysis (DTA) at a heating rate of 20 °C min−1. The bulk alloys were annealed at slightly below the L21 ↔ B2 order–disorder temperature. The constituent phases in
Bulk alloys
Fig. 1a shows the XRD patterns of Co2Fe(GaxGe1−x) alloy powders for x = 0, 0.25, 0.5, 0.75 and 1. It clearly shows that a certain degree of L21 order exists in all the Co2Fe(GaxGe1−x) samples. Note that Balke et al. [19] reported that the characteristic (1 1 1) and (2 0 0) reflections of the L21 structure were not observed in the XRD partterns of the Co2FeGe and Co2FeGa alloys and employed the extended X-ray absorption fine structure technique to show the existence of L21 order. However, our XRD results
Discussion
Earlier ab initio calculations on Co2FeGe and Co2FeGa did not predict these were half-metals [18], [19], [20]. Our results, which consider the on-site correlations of Fe in the Y site in the X2YZ L21 lattice and the Hubbard parameter U, which were not considered by the earlier reports [18], [19], [20], suggest that Co2FeGe could be half-metal. However, the current spin polarization of the Co2FeGe alloy measured by PCAR was only 0.56, which is lower than that for Co75Fe25 (P ∼ 0.58) [29]. XRD and
Conclusion
The structure, magnetization and spin polarization of a new series of Co2Fe-based Heusler alloys, Co2Fe(GaxGe1−x) (0 < x < 1), were investigated. The quaternary alloys exhibited L21 order in the as-cast as well in the annealed conditions. The intrinsic spin polarization of the quaternary alloys measured using the PCAR technique was found to be as high as 69% for x = 0.5, whereas the ternary alloy showed much lower spin polarization. Ab initio calculations performed with GGA + U potentials showed that
Acknowledgement
This work was supported by the Grant-in-Aid for Scientific Research (A) 22246091.
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