Materials Transactions, Vol. 47, No. 1 (2006) pp. 11 to 14 Special Issue on Present Status of the Research on Ordered Alloys and the Application to Magnetic Devices #2006 The Japan Institute of Metals Uncompensated Spin Elements in Ferromagnetic and Antiferromagnetic Bilayer with Non-Collinear Spin Structure Chiharu Mitsumata1 , Akimasa Sakuma2 , Kazuaki Fukamichi3 and Masakiyo Tsunoda4 1 Advanced Electronics Research Laboratory, Hitachi Metals Ltd., Kumagaya 360-0843, Japan Deptartment of Applied Physics, Graduate School of Engineering, Tohoku University, Sendai 980-8579, Japan 3 Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, Sendai 980-8577, Japan 4 Department of Electronic Engineering, Graduate School of Engineering, Tohoku University, Sendai 980-8579, Japan 2 The exchange bias in a ferromagnetic (FM) and antiferromagnetic (AFM) bilayer with a -phase disordered structure has been investigated within a framework of Heisenberg model. The magnetic atoms in the AFM layer realize the triple Q structure due to geometrical spin frustrations. This non-collinear spin structure can bring about an exchange bias in the FM/AFM bilayer system. Under the influence of the exchange bias, the uncompensated spin element appears in the AFM layer, accompanied by a shifted loop in magnetization curves, in accord with the measured loop by X-ray magnetic circular dichroism spectroscopy for an AFM layer. (Received August 5, 2005; Accepted September 8, 2005; Published January 15, 2006) Keywords: antiferromagnetic, exchange bias, exchange coupling, spin frustration, spin structure, non-collinear spin, Heisenberg model 1. Introduction The exchange bias in a ferromagnetic (FM) and antiferromagnetic (AFM) bilayer system plays a key role in enabling high density in magnetic storages. FM/AFM bilayer systems are attractive in spin valve heads and perpendicular recording media to control magnetic domains. For such FM/AFM bilayer systems, a variety of AFM materials have been investigated, and many models for the exchange bias have been proposed.1,2) Several kinds of AFM materials have a non-collinear spin structure.3) It should be noted, however, that the proposed conventional models discuss the collinear spin structure only. Therefore, we have focused the noncollinear spin structure in the AFM alloy, and shed light on the mechanism of its exchange bias.3–5) Recently, the domain observation by X-ray magnetic circular dichroism (XMCD) spectroscopy for AFM materials becomes very important to investigate the exchange bias in FM/AFM systems. In general, the summation of AFM spin vectors shows zero, and that cancellation of spins is called ‘‘the compensated state’’. On the other hand, as a result of the summation of spin vectors, the uncompensation stands for the generation of finite spin elements. The uncompensated spin in the domain state model was predicted by Nowak et al.6) Such uncompensated spin elements in AFM layers were actually found in a Mn–Ir/Co system by Ohldag et al.7) It was considered that the interfacial roughness forces an unbalance in the number of spins on AFM sub-lattice. The collinear spin structure in AFM layers has been formed the base of the physical aspect of the domain state model. However, it should be emphasized that the spin structure for several kinds of -phase disordered alloys is not collinear.3) In the present paper, we discuss the appearance of the non-collinear spin structure in the -phase disordered AFM alloy, and investigate the uncompensated spin state at the interface of FM/ AFM bilayer system. 2. Calculation Method of the Present Model The present model works within the framework of the classical Heisenberg model. In order to define the magnetic structure in the AFM/FM bilayer, the following Hamiltonian described in eq. (1) is evaluated in the numerical calculations. X X J1;i; j hSi S j i J2;i;k hSi Sk i H¼ hi; ji X i hi;ki AðSi Þ gB X hSi H app i ð1Þ i where Si is the unit vector of the spin at the ith atom, and the summation is carried out over all possible spin pairs by using the exchange constants, J1 and J2 . The indices j and k denote the first and second nearest neighboring spins, respectively. The third and forth terms in eq. (1) describe the magnetic anisotropy energy and the Zeeman energy, respectively. Here, the function AðSi Þ stands for the magnetic anisotropy energy, and the vector H app represents the applied field. When spin Si belongs in the FM layer, the anisotropy energy can be expressed AðSi Þ ¼ Du hSi ni2 , where Du and the unit vector n respectively stand for the anisotropy constant and the easy axis direction. In the present case, the vector n points out ½01 1 direction. On the other hand, when spin Si belongs in the AFM layer, the magnetic anisotropy function can be AðSi Þ ¼ D1 ð2b 2c þ 2c 2a þ 2a 2b Þ þ D2 2a 2b 2c , where D1 and D2 denote the second and fourth orders of magnetic anisotropy constants in the AFM layer, respectively. Also, a , b , and c designate the elements of the spin vector Si in the directions of the a-, b-, and c-axes in the -phase alloy, respectively. In the AFM layer, the face centered sites in the fcc lattice are randomly occupied by magnetic atoms and non-magnetic atoms, composing a -phase disordered alloy. The atomic configuration of the present model is illustrated in Fig. 1. The bilayer is stacked to the h111i orientation, and the thickness of FM and AFM layers are 9 monolayers (MLs) and 100 MLs, respectively. The thickness of 100 MLs corresponds to 18 20 nm in representative Mn-based alloys. 12 C. Mitsumata, A. Sakuma, K. Fukamichi and M. Tsunoda [111] FM 9 ML φ θ = cos −1 2 / 3π [011] θ [101] AFM 10 − 100 ML θ J1 J2 φ Magnetic Non-magnetic FM atom φ = π/2 Binary AFM alloy Fig. 1 The atomic configuration near the interface of the AFM/FM bilayer model. For the sake of simplicity, the values of J1 are assumed to be 20 meV in the FM layer and 20 meV in the AFM layer, respectively. The exchange constants J2 is defined by J2 ¼ jJ1 j=2.8) J1 at the interface is assumed to be equivalent to J1 in the AFM layer. These exchange constants give the Néel temperature TN ¼ 695 K, which roughly agrees with TN of the -phase disordered Mn-based alloys (Mn–Ir, Mn–Rh, etc.).3) The anisotropy constant D is assumed to be Du =J1 ¼ 3 106 in the FM layer and D1 =J1 ¼ D2 =J1 ¼ 3 103 in the AFM layer, respectively.5) The magnetization process is solved by using the following motion equation of spin within the scheme of a forward difference method; dS ¼ ðS H eff Þ fS ðS H eff Þg; dt ð2Þ where and are the gyromagnetic and damping constants, respectively. The effective field H eff is obtained by the derivation of Hamiltonian (1). 3. Results and Discussion The spin structure of -phase alloy is illustrated in Fig. 2 in which 75% of magnetic atoms and 25% non-magnetic atoms are included in the unit cell. As seen from this figure, the AFM alloy realizes a triple Q (3Q) spin structure where an angle between AFM spins indicates cos1 ð1=3Þ, showing a typical non-collinear spin configuration. The 3Q spin structure can be generated by spin frustrations caused by the geometry of magnetic atoms in the -phase disordered structure. The calculated spin structure is provided by the single spin flip Metoropolis scheme in the Monte Carlo simulation. Also, the theoretical approach with a quantum spin predicts the generation of the 3Q structure in AFM spins on an fcc lattice.9) For the AFM spins, four equivalent atoms are composed in the unit cell, and the summation of those spins should become zero in the ground state. For the h111i stacking of the FM/AFM bilayer, the (111) plane of the AFM layer faces to the FM layer. In the case of (111) surface of the -phase AFM alloy, the spin configuration can be compensated where the summation of AFM spins is expected to becomes Si ¼ 0. On the other hand, in the case of interface in the FM/AFM Fig. 2 The spin structure of the -phase disordered AFM alloy. 75% of magnetic atoms and 25% of non-magnetic atoms are included. bilayer, the uncompensated spin element of the AFM layer needs to remain at the interface at least, because of the finite coupling energy at the interface as following. The coupling energy at the FM/AFM interface is given as X JI hSFM SAFM i: ð3Þ EI ¼ Since, all FM spins SFM are equivalent vectors, eq. (3) can be rewritten as D E X EI ¼ JI SFM SAFM : ð4Þ At the interface preferring the h111i orientation, the coupling energy becomes zero from P eq. (4), if the summation of AFM spins SAFM becomes SAFM ¼ 0. However, the exchange coupling bias is actually observed in thePh111i stacked bilayer.10) Accordingly, the condition of SAFM 6¼ 0 is required for the (111) interface. The exchange coupling between the FM and AFM layers influences the relaxation of the direction of spins. The spin configuration near the interface when the 3Q spin structure is realized in the -phase disordered AFM layer is shown in Fig. 3(a). The indices of the AFM spins represent the equivalent atomic sites. The ground state of 3Q spins is illustrated in Fig. 3(b), in which the angle between AFM spins is cos1 ð1=3Þ. The direction of the AFM spin near the interface is different from that of the ground state. The relaxation of spins influences the deviation of angles between the AFM spins. Consequently, the resultant spin element becomes finite, forming the uncompensated spins in the AFM layer. The appearance of uncompensated spins was reported by Nowak et al.6) within the scheme of Ising spin model based on an interfacial roughness to retain the uncompensated spin component. On the contrary, in the present model, no roughness is also able to create the uncompensated spin element. Consequently, the frustration of spins at the interface could realize a finite value of the magnetization in the AFM layer. Such uncompensated spin element is quite small, but can be observed by X-ray magnetic circular dichroism (XMCD) spectroscopy.7) The characteristics of magnetization in the AFM layer shows a shifted loop both in the field and magnetization axes of M–H loops in the XMCD measurements,7) when the magnetization loop in the FM layer is shifted by the bias field. Uncompensated Spin Elements in Ferromagnetic and Antiferromagnetic Bilayer with Non-Collinear Spin Structure On the other hands, there is no loop shift in the AFM layer when the magnetization loop in the FM layer is not shifted. The calculated corresponding magnetization loops are shown in Fig. 4. The magnetization m is obtained by the average of all the AFM or FM spins. The average of the AFM spins includes all equivalent atomic sites shown in Fig. 3. The thickness of the AFM layer is adopted for 10 and 100 MLs in Figs. 4(a) and (b), and in Figs. 4(c) and (d), respectively. The thickness of the FM layer is 9 MLs in both the cases. [111] [011] [101] (a) (b) IV III I IV II III II I Unit cell FM spin AFM spin 1.5 1.0 0.5 0.0 -0.5 -1.0 -1.5 Magnetization (m/ms) 1.5 1.0 0.5 0.0 -0.5 -1.0 -1.5 (a) -6 -4 -2 0 2 4 Applied field (H/D) 6 (c) -6 0 2 4 -4 -2 Applied field (H/D) For the thin AFM layer (10 MLs), the magnetization loop in the FM layer exhibits a symmetric switching field, giving no exchange bias as seen from Fig. 4(a). The resultant magnetization in the AFM layer shows a finite value. Such uncompensated spin element forms the hysteresis loop corresponding to the magnetization loop in the FM layer. The switching field in the AFM layer is equivalent to that in the FM layer. On the other hand, in the case of thick AFM layer (100 MLs), the FM spins show a shifted magnetization loop under the influence of the exchange bias in Fig. 4(c). In the AFM layer, at the same time, the resultant spin vector becomes finite, forming an uncompensated spin element, as well as spins in the thin AFM layer. The uncompensated spin element in the AFM layer shows a hysteresis loop in a similar manner as the FM layer, and it also indicates the biasing shift in the direction of the abscissa (field axis) in Fig. 4(d). The biasing field in the AFM layer is equivalent to the bias in the FM layer. Consequently, the exchange bias influences the loop shift in both the FM and AFM layers, and the agreement between such bias values of the FM and AFM layers could reproduce the measured results in XMCD spectroscopy.7) The sign of resultant spin in the AFM layer is dominated by the exchange constant J1 at the interface. In the present model, J1 < 0 is assumed, although the positive J1 at the interface reverses the sign of resultant spin in Fig. 4(d), because the uncompensated spin element is sensitive to the exchange interaction at the interface. For example, the depth profile of uncompensated spin elements was not uniform in the case for the L12 -type ordered AFM layer.11) The depth profile of uncompensated spins in -phase AFM layer will be discussed in a separate paper. Magnetization (m/ms) Magnetization (m/ms) Magnetization (m/ms) Fig. 3 The spin configuration of the AFM/FM bilayer. (a) The spin configuration near the interface, (b) the ground state of the spin structure in the magnetic unit cell. 6 13 0.03 0.02 0.01 0.00 -0.01 -0.02 -0.03 -6 (b) -4 -2 0 2 4 Applied field (H/D) 6 0.003 0.002 0.001 0.000 -0.001 -0.002 -0.003 -6 (d) -4 -2 0 2 4 Applied field (H/D) 6 Fig. 4 The magnetization loops in the AFM/FM bilayer system. (a) The magnetization in the FM layer with the thin AFM layer, (b) the resultant magnetization in the thin AFM layer with the thickness of 10 MLs, (c) the magnetization in the FM layer with the thick AFM layer, (d) the resultant magnetization in the thick AFM layer with the thickness of 100 MLs. The resultant magnetization is averaged all over the AFM layer. 14 C. Mitsumata, A. Sakuma, K. Fukamichi and M. Tsunoda In Fig. 4, the asymmetry between the positive and negative value of resultant magnetization is determined by the following eq. (5), ¼ ðmpos þ mneg Þ=ðmpos mneg Þ: ð5Þ where mpos and mneg are the resultant magnetizations in the remanent state of AFM layers. The calculated value of asymmetry in the AFM layer becomes 10 ML ¼ 0 in Fig. 4(b). Thus, in the case of no exchange bias, a loop shift in the ordinate (magnetization axis) is not obtained. Meanwhile, in Fig. 4(d), the value of asymmetry shows 100 ML ¼ 0:19. Namely, the asymmetry 100 ML is significantly larger than 10 ML in the calculation of magnetization process. The finite value of asymmetry gives a loop shift downward in the ordinate. Consequently, in both the thin and thick cases, the calculated loops would reproduce the XMCD measurements. 4. Conclusion The magnetic structure and the magnetization process of AFM/FM bilayer are calculated within the framework of classical spin model. For the -phase disordered alloy in the AFM layer, the uncompensated spin element is generated due to the frustration of spins, which appears to be independent of the AFM thickness. Such uncompensated spin results in a hysteresis loop corresponding to the magnetization loop of the FM layer. For the thick AFM layer, the loop of uncompensated spin element is shifted in both directions of the applied field and the magnetization. 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