# Structural Dependent Ferromagnetic-Nonmagnetic Phase Change in FePtRu Films

Authors: Takashi Hasegawa; Kosuke Ito
Journal: Advances in Materials Science and Engineering
 (2017)

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## Abstract

Herein, we studied correlations between crystal structures and magnetic properties of FePt1−xRux films. At room temperature, the chemical disordered A1 films with 0≤x<0.20 and 0.20≤x≤1.00 exhibited ferromagnetic properties and paramagnetic properties, respectively. Curie temperature of the disordered film with x=0.30 was 200 K. In contrast, the ordered L10 films had ferromagnetic properties in a wider range of 0≤x<0.80 with the magnetic easy-axis perpendicular to the film plane. For 0≤x≤0.50, with the ordered structure, the films had high magnetization and high uniaxial magnetic anisotropy of over 107 erg cm−3. For x = 0.60–0.70 with the ordered structure, a temperature-dependent magnetic phase transition appeared, and magnetization reached its maximum value at around 200 K. Using this material system, we proposed a nanopatterning method involving a ferromagnetic-paramagnetic phase change due to the ordered-disordered structural transformation.


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## Body

## 1. Introduction

Increased power consumption in data centers having millions of hard disk drives (HDDs) has emerged as a serious issue. Decreasing the number of HDDs by increasing their magnetic storage density can be a simple and efficient means to mitigate increased power consumption. Ferromagnetic (FM) thin films prepared using nanofabrication techniques can be used for high-density magnetic data storage [1–3] and spintronic devices [4].Bit-patterned media (BPM) is a candidate for the creation of ultra-high-density magnetic data storage devices [1, 2]. BPM consist of multiple phases, which include the FM phase (dots) characterized by a high uniaxial magnetic anisotropy along with, in principle, diamagnetic, antiferromagnetic (AF), and paramagnetic (PM) phases. Ion milling is conventionally used for nanofabrication of two-dimensional FM films [5, 6], which produces physically separated FM regions. After ion milling, backfill and polishing stages are required to obtain BPM with smooth surfaces, which is a prerequisite for read/write heads to be able to fly at a few nanometers above the medium surface [1].Another BPM fabrication method, using ion irradiation, has also been proposed [7, 8]. This method can replace the three processes of ion milling, backfill, and polishing steps, thereby streamlining the production of BPM. Ion irradiation results in structural disordering. Co/Pt multilayers [7, 8] and L10 CrPt3 films [9] with an uniaxial magnetocrystalline anisotropy constant (Ku) of ~106 erg cm−3, which is not sufficient for the realization of high magnetic data storage density of over 2 Tb in−2, are transformed from FM to PM phase after ion irradiation.A problem faced by high-density magnetic data storage is the thermal fluctuation effect of magnetic grains or dots. The magnetic anisotropy energy (KuV; V: volume of an isolated magnetic grain or dot) becomes lower relative to the thermal fluctuation energy (kBT; kB: Boltzmann constant, T: temperature) when the grain and/or dot size is reduced for increasing storage density. The thermal fluctuation can be sufficiently reduced using materials with high Ku, satisfying the thermal stability factor requirement of (KuV/kBT) > 60 (this metric was derived using the Sharrock equation [10]) which is typically regarded as a minimum requirement for magnetic data storage [1, 11].L
1
0 FePt (CuAu-I type, fct, a=b>c) films with ordered structures are possible candidates for BPM due to their high Ku of 7.0 × 107 erg cm−3, high saturation magnetization (Ms) of 1100 emu cm−3, high corrosion resistance, and low resistivity [12–14], which leads to excellent thermal stability of magnetization in nanometer-size structures. After ion irradiation, the ordered L10 FePt films undergo transformation from the hard-FM phase (high Ku) to the soft-FM phase (low Ku) with the disordered A1 structure (fcc, a=b=c) [15–20]. Although the L10 FePt is suitable for BPM, modifying its properties using ion irradiation is difficult due to the insensitivity of magnetization with ion irradiation. The high spontaneous magnetization (M0) of the soft-FM region (interdot spacing), wherein the ions are irradiated, leads to spike noise in the storage media. Therefore, developing high-Ku and high-Ms materials, whose Ku and Ms values decrease upon ion irradiation with high sensitivity, is required.In our previous study, nonmagnetic phases were observed by replacing Fe with Mn [21] and Pt with Rh [22] in FePt films, and the former improved the sensitivity of Ms to ion irradiation. The L10 Fe1−xMnxPt films with x≤0.44 exhibit FM properties corresponding to Ku> 2.1 × 107 erg cm−3, whereas, disordered A1 films with x≥0.44 possess PM properties at room temperature. These films change from a FM to PM state as the L10 structure transforms into the A1 structure due to ion irradiation. However, the high Mn contents could decay corrosion resistance and Ku. By replacing Pt with Ru in the L10 FePt films, which could be uninfluential to its corrosion resistance, a reduction of Curie temperature (Tc) has been reported [23].In this study, by replacing Pt with Ru inA1 and L10 FePt films, correlations between crystal structures and magnetic properties were investigated.


## 2. Materials and Methods

Fe50(Pt1−xRux)50 films with the thickness of 6.0 nm were deposited by magnetron cosputtering at a base pressure of 10−5 Pa using Ar gas at 0.5 Pa on a single-crystalline MgO (100) substrate at 298 K. The Ru composition (x) was controlled by varying the sputtering rates of the Pt and Ru targets and was detected using an electron probe X-ray microanalyzer. The films were annealed by rapid thermal annealing (RTA) with a heating rate of 300 K s−1 under a vacuum of 2 × 10−4 Pa. The crystalline structure was studied using out-of-plane X-ray diffraction (XRD) measurement and in-plane XRD measurement with CuKα radiation. A vibrating sample magnetometer (VSM) with a maximum field of 18 kOe and a superconducting quantum interference device (SQUID) magnetometer with a maximum field of 50 kOe were used to assess the magnetic properties of the films.


## 3. Results and Discussion

Figure1(a) shows out-of-plane XRD patterns for the as-deposited FePt1−xRux films of thickness 6.0 nm. The Ru composition x of the FePt1−xRux films was changed from 0 to 1.00 and is shown from 0 to 0.30 with the background pattern (sample holder and substrate) in the figure. Only the background peaks were observed for all the films, since the fundamental (111) reflection peaks for the disordered A1 structure appear at the same angle as the MgO (100) substrate.Figure 1
Crystal structure and magnetic properties of disorderedA1 FePt1−xRux films before annealing (as-deposited films). (a) Out-of-plane XRD patterns. Magnetization curves of the films with x = (b) 0, (c) 0.10, (d) 0.20, and (e) 0.30. Magnetic fields (H) were applied perpendicular (⊥, dashed line) and parallel (//, solid line) to the film plane at 298 K. (f) Temperature dependence of magnetization (M-T curve) for the film with x = 0.30, measured from 300 K to 30 K with a field of 1 kOe applied parallel to the film plane after saturation. (g) x-dependence of M0 at 298 K.Figures1(b)–1(e) show magnetization curves of the films with x = 0, 0.10, 0.20, and 0.30, measured by the VSM with a maximum field of 18 kOe applied perpendicular (⊥, dashed line) and parallel (//, solid line) to the film plane at 298 K. The magnetic easy-axes of all the films are parallel to the film plane. Figure 1(f) shows the temperature (T) dependence of magnetization (M) (M-T curve) for the film with x=0.30 at temperatures at or below room temperature (300 K down to 30 K), measured using a SQUID magnetometer with a field of 1 kOe applied parallel to the film plane after saturating the magnetization by a field of 50 kOe at 298 K. M decreases with an increase in T and approaches 0 at around Tc of 200 K. Tc was estimated from the M2-T curve (not shown). This indicates that the film with x=0.30 is in the PM phase at room temperature.Thex-dependence of M0, determined using the Arrott plot [24] at 298 K, is shown in Figure 1(g). M0 decreases with increasing x, and an abrupt decrease in M0 is found at x=0.20, caused by the decrease in Tc. This implies that the films with 0≤x<0.20 are in the FM phase, and the films with x≥0.20 are in the PM phase at room temperature.Figures2(a) and 2(b) show out-of-plane XRD patterns and in-plane XRD patterns, respectively, for the FePt1−xRux films after annealing at 1173 K for 4 h with a heating rate of 300 K s−1 by RTA. In Figure 2(a), only superlattice (001) and fundamental (002) reflection peaks for the ordered L10 structure are observed for the films with 0≤x≤0.70, whereas only background peaks were observed for the films with 0.80≤x≤1.00 due to overlapping of the fundamental (111) reflection peak for the disordered A1 structure and the reflection peaks for the MgO (100) substrate. In Figure 2(b), only the fundamental (200) reflection peak is observed for the films with 0≤x≤0.60, whereas only background peaks are observed for the films with 0.70≤x≤1.00. These reflection patterns indicate that the (001) crystalline texture is normal to the film plane in the films with 0≤x≤0.70, whereas the disordered A1 structure is obtained in the films with 0.80≤x≤1.00. This result is broadly consistent with the previous report [23]. The degrees of long-range chemical order parameter were estimated to be ~0.90 in the films with 0≤x≤0.60.Figure 2
Crystal structure of FePt1−xRux films after annealing at 1173 K for 4 h. (a) Out-of-plane XRD patterns and (b) in-plane XRD patterns. (c) Lattice constants (a, c, and c/a) as a function of x.The lattice constants (a, c, and c/a) are plotted as functions of x in Figure 2(c). c and a values were obtained from the out-of-plane and in-plane XRD measurements, respectively. a and c values of the film with x = 0 are about 0.3867 nm and 0.3726 nm, respectively, and are close to those of the FePt bulk alloy (a = 0.3852 nm, c = 0.3713 nm; PDF number 43-1359). The values of a are ~0.39 nm for each x which could be kept by the epitaxial growth, whereas c and the axial ratio (c/a) values decrease with increasing x. By considering the layer-by-layer atomic configuration in L10 FePt and the differences of atomic radiuses of Pt, Ru, and Fe (Pt > Ru > Fe), the decrease in the lattice constant c indicates the substitution of Ru for Pt.Figures3(a)–3(e) show magnetization curves of the films with x = 0, 0.10, 0.20, 0.40, and 0.60, measured by the SQUID magnetometer with a maximum field of 50 kOe applied perpendicular (⊥, filled symbols) and parallel (//, open symbols) to the film plane at 298 K. The magnetic easy-axes of all the films were perpendicular to the film plane. Ku values were evaluated using the magnetization curves [25]. The magnetic anisotropy field (Hk) was determined from the intersection point of the extrapolated magnetization curves of the magnetic fields applied parallel and perpendicular to the film plane. Only the linear part of the in-plane magnetization curve was extrapolated. Consequently, Ku was obtained using the relation Ku=(Ms×Hk/2)+Kshape, where Kshape is the shape anisotropy calculated using the demagnetization factors (N) of the film shape (N⊥=4π, N//=0). The films with 0≤x≤0.50 have high magnetization of 500≤M0≤800 emu cm−3, high coercivity of 15≤Hc≤43 kOe, and high anisotropy of 2.6 × 107 ≤Ku≤ 5.0 × 107 erg cm−3 in the perpendicular direction, and these results are broadly consistent with the previous report [23].Figure 3
Magnetic properties of the FePt1−xRux films after annealing at 1173 K for 4 h. Magnetization curves of the ordered L10 FePt1−xRux films with x = (a) 0, (b) 0.10, (c) 0.20, (d) 0.40, and (e) 0.60. H was applied perpendicular (⊥, filled symbols) and parallel (//, open symbols) to the film plane at 298 K. (f) x-dependence of M0 and Ku at 298 K.Thex-dependence of M0 and Ku is plotted in Figure 3(f). M0 and Ku decrease with increasing x and reach almost 0 at x=0.80, which is the critical composition for the transition from the L10 structure to the A1 structure. For instance, L10 film with x=0.20 has FM properties with a Ku = 3.5 × 107 erg cm−3, whereas, the disordered A1 film with x=0.20 has PM properties at room temperature. The film can change from a FM to PM state as the L10 structure transforms into the A1 structure due to ion irradiation. By using the thermal stability factor (KuV/kBT) > 60 and Ku=3.5×107 erg cm−3, the smallest diameter of the spherical shape was estimated to be ~5.1 nm, which indicates that this material system has sufficient thermal stability for use in high-density magnetic data storage media of ~10 Tb in−2.Figures4(a)–4(d) show the M-T curves of the films with x = 0.20, 0.40, 0.60, and 0.80 at temperatures at or below room temperature (300 K down to 30 K), measured using the SQUID magnetometer with a field of 1 kOe applied perpendicular to the film plane after saturating the magnetization by a field of 50 kOe at 298 K. In the films with x≤0.40, M increases with a decrease in T due to the typical FM properties. However, at x=0.60, M reaches its maximum value at 210 K (T0) and decreases with a decrease in temperature below T0. This indicates that the film with x=0.60 can contain an antiferromagnetically ordered phase (spin-glass or canted-AF etc.) at temperatures below T0. In the films with x≥0.80, M is almost 0 at each T. These results imply that the films with 0≤x≤0.40 should have the FM–PM transition above 300 K, the films with 0.40<x<0.80 have the antiferromagnetically ordered phase FM-PM transition, and the films with 0.80≤x≤1.00 have the FM-PM transition below 300 K due to the A1 structure.Figure 4
Temperature dependence of magnetization (M-T curves) for the FePt1−xRux films after annealing at 1173 K for 4 h with x = (a) 0.20, (b) 0.40, (c) 0.60, and (e) 0.80, measured from 300 K to 30 K with a field of 1 kOe applied perpendicular to the film plane after saturating.Finally, we propose a nanopatterning method for this material system. According to our previous results, the orderedL10 structures of FePtX were easily transformed to the disordered A1 structure under ion irradiation [15–21]. Figure 5 shows the schematics of a nanopatterning method using an FM–PM phase change due to the L10–A1 structural transformation caused by ion irradiation. After ion irradiation, FM dots having L10 structure should be surrounded by PM spacing having A1 structure with a smooth disc surface.Figure 5
Schematics of the nanopatterning method using FM-PM phase change.


## 4. Conclusions

Correlations between crystal structures and magnetic properties of FePt1−xRux films (6.0 nm thick) were investigated.(1) Magnetic properties ofA1 disordered structure (as-deposited films): M0 decreased with increasing x, and an abrupt decrease in M0 was found at x=0.20 at room temperature, due to the decrease in Tc. In the range of 0≤x<0.20, the films had FM properties (100≤M0≤1050 emu cm−3) with their magnetic easy-axes parallel to the film plane. In the range of x≥0.20, the films had PM properties (M0≈0 emu cm−3) at room temperature.(2) Magnetic properties ofL10 ordered structure (annealed films): M0 and Ku decreased with increasing x. In the range of 0≤x≤0.50, the films had FM properties (500≤M0≤800 emu cm−3, 15≤Hc≤43 kOe, 2.6 × 107 ≤  Ku  ≤ 5.0 × 107 erg cm−3), with their magnetic easy-axis perpendicular to the film plane. In the range of 0.40<x<0.80, the films could contain an antiferromagnetically ordered phase at temperatures below room temperature.For instance, theL10 film with x=0.20 had FM properties with a Ku = 3.5 × 107 erg cm−3, whereas the disordered A1 film with x=0.20 had PM properties at room temperature. The film could change from a FM to PM state as the L10 structure transforms into the A1 structure due to ion irradiation. These results suggest the possibility of applying the material system for nanopatterning method for high-density magnetic storage media.



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*Source: 8949458-2017-07-04.xml*