Heusler合金Co2FeAlxSi1–x跨尺度结构有序度调控及其对磁致伸缩性能的影响

姚亮; 芦光辉; 杜杰; 刘永昌; 郗学奎; 王文洪

doi:10.7498/aps.74.20250358

摘要
本文通过实验系统研究了Heusler合金Co₂FeAl_xSi_1–x (x = 0, 0.25, 0.5, 0.75, 1)体系中原子占位有序度与磁致伸缩的关联机制. 研究发现, Al掺杂可导致体系从高度有序的L2₁结构向B2无序结构转变, 并在x = 0.25—0.5时诱导L2₁/B2两相共存界面态的形成, 此时有序度计算结果显示S_L21/S_B2 = 0.5—0.9. 实验结果表明, 这种界面态的出现显著增强了饱和磁致伸缩系数并在过渡到B2结构后再次减小. 该结果定量揭示了原子的局部无序占位可通过降低立方对称性、引入局域晶格畸变并改变磁畴结构, 从而提升磁弹耦合的物理机制. 本研究报道了12种Co基Heusler合金的磁致伸缩系数, 其中Co₂MnGa和Co₂CrGa展现出优于其他Co基Heusler合金的潜力, 填补了该体系磁致伸缩性能参数的空白, 并验证了该多晶材料的线性正磁致伸缩特性; 提出了基于原子占位有序度调控的磁致伸缩性能优化策略, 为开发耐高温、高自旋极化率的磁致伸缩材料提供了新方向.

关键词:
Co基Heusler合金 /

有序度 /

结构相变 /

磁致伸缩
Abstract
Co-based Heusler alloys have emerged as highly promising systems within the Heusler alloy family due to their high Curie temperatures and potential half-metallicity. Since the concept of half-metallic ferromagnets is proposed, these alloys have attracted significant attention because of their high spin polarization, excellent magnetic performance, and thermal stability. The existing studies predominantly focus on spin-transport properties, but systematic studies on their magnetostriction remain scarce. The electronic structure and magnetism of Co-based Heusler alloys are critically dependent on atomic-site ordering: their spin polarization, Curie temperature, and magnetocrystalline anisotropy are closely related to crystal structure, such as L2₁ and B2. A highly ordered L2₁ structure is essential for maintaining half-metallicity, as structural disorder can induce significant changes in electronic hybridization and exchange interactions, thereby significantly changing macroscopic magnetism. Additionally, ordering control is also expected to modulate magnetostriction by modifying lattice symmetry and local distortions. Notably, in Fe–Ga alloys, disorder engineering has been employed to induce local short-range order and lattice distortion, thereby enhancing magnetostriction, a mechanism that may similarly operate in Co-based systems. However, the higher lattice symmetry and stronger orbital hybridization in these alloys can lead to fundamentally distinct mechanisms, which needs to be validated experimentally. This study focuses on the Co₂FeAl_xSi_1–x system to systematically probe the relationship between composition-driven structural evolution (i.e., L2₁ to B2 transition) and magnetostrictive performance through adjusting Al/Si ratio. The study aims to clarify the correlation between composition-induced structural evolution and magnetostrictive behavior, thereby revealing the regulatory role of atomic ordering in magnetoelastic coupling and providing theoretical insight for designing high-performance magnetostrictive materials.The correlation between atomic site ordering and magnetostriction in Heusler alloy Co₂FeAl_xSi_1–x (x = 0, 0.25, 0.5, 0.75, 1) is systematically investigated in experiment. The results reveal that Al doping drives a structural transition from the highly ordered L2₁ phase to the disordered B2 phase, inducing a coexisting L2₁/B2 interface state at x = 0.25–0.5, with the calculated ordering parameters S_L21/S_B2 ranging from 0.5 to 0.9. The experimental data demonstrate that this interface state significantly enhances the saturation magnetostriction coefficient (λ_s), which subsequently decreases as it further transitions to the B2-dominated structure. These findings quantitatively clarify the physical mechanism by which local atomic disorder enhances magnetoelastic coupling through reducing cubic symmetry, localizing lattice distortion, and changing magnetic domain configuration. Furthermore, this study reports for the first time the magnetostriction coefficients of 12 Co-based Heusler alloys, among which Co₂MnGa and Co₂CrGa exhibit superior potential compared with other Co based Heusler alloys, filling the gap in magnetostriction performance parameters of this system. The linear positive magnetostriction behaviors of the polycrystalline materials are also validated. This study provides a strategy for optimizing magnetostriction performance through atomic site ordering control, and points out a new direction for the development of magnetostrictive materials with high-temperature stability and high spin polarization.

Keywords:
co-based Heusler alloy /

atomic ordering /

structural phase transition /

magnetostriction
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图 1 (a) Co₂FeAl_xSi_1–x的晶体结构(L2₁结构和B2结构); (b) Co₂FeAl_xSi_1–x样品的粉末XRD图谱; (c) Co₂FeAl_xSi_1–x样品的晶格常数随Al含量x的变化关系

Fig. 1. (a) Crystal structure of Co₂FeAl_xSi_1–x(L2₁ structure and B2 structure); (b) powder XRD patterns of Co₂FeAl_xSi_1–x; (b) variation of lattice constant with Al content x in Co₂FeAl_xSi_1–x.

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图 2 Co₂FeAl_xSi_1–x样品退火1 d (a)和7 d (b)的粉末XRD图谱; (c)—(e)退火前后样品的有序度S_L21和S_B2随Al含量x的变化关系　　　　

Fig. 2. (a), (b) Powder XRD patterns of Co₂FeAl_xSi_1–x annealed for 1 day and 7 days; (c)–(e) variation of ordering degrees S_L21 and S_B2 with Al content x before and after annealing.

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图 3 (a) 3种不同有序态的磁致伸缩曲线; (b) Co₂FeAl_xSi_1–x退火前后的磁致伸缩应变λ随Al含量x的变化关系

Fig. 3. (a) Magnetostriction curves of three different ordered states; (b) variation of magnetostriction λ_s with Al content x in Co₂FeAl_xSi_1–x before and after annealing.

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图 4 (a) Co₂FeAl_xSi_1–x的磁致伸缩应变λ随S_L21的变化关系; (b) Co₂FeAl_xSi_1–x的磁致伸缩应变λ随S_L21/S_B2的变化关系

Fig. 4. (a) Variation of magnetostriction λ with S_L21 and S_B2 in Co₂FeAl_xSi_1–x; (b) variation of magnetostriction λ with S_L21/S_B2 in Co₂FeAl_xSi_1–x.

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图 5 Co₂FeAl_xSi_1–x的(a)M-H曲线与(b)磁致伸缩曲线

Fig. 5. (a) M-H and (b) magnetostriction of Co₂FeAl_xSi_1–x.

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图 6 多晶材料转角磁致伸缩测量示意图

Fig. 6. Schematic diagram of the rotational magnetostriction measurement for polycrystalline materials.

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图 7 Co₂FeAl_xSi_1–x的磁致伸缩应变λ随θ的变化关系

Fig. 7. Variation of magnetostriction λ with θ in Co₂FeAl_xSi_1–x.

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表 1 部分Co基Heusler合金的晶格常数a, 居里温度T_c, 自旋极化率P ^[34–53]与磁致伸缩系数λ_s

Table 1. Lattice constant a, Curie temperature T_c, spin polarization P^[34–53], and magnetostriction λ_s of selected co-based heusler alloys.

成分	a/Å	T_c/K	P/%	λ_s/ppm
Co₂FeSi	5.645	1100	57	22
Co₂FeAl	5.728	1170	58	21
Co₂FeGa	5.737	1056	59	24
Co₂VGa	5.792	357	75	13
Co₂CrAl	5.887	334	62	8
Co₂CrGa	5.765	495	61	42
Co₂MnAl	5.749	693	59	14
Co₂MnGa	5.767	694	55	45
Co₂MnSi	5.654	985	56	18
Co₂MnGe	5.749	905	58	25
Co₂MnSn	5.984	829	60	20
Co₂MnSb	5.943	600	50	8

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Heusler合金Co₂FeAl_xSi_1–x跨尺度结构有序度调控及其对磁致伸缩性能的影响

Control of cross-scale f structural order of Heusler alloy Co₂FeAl_xSi_1–x and its influence on magnetostrictive properties

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