Structural and magnetic properties
Vicinal substrates denote those substrates with periodic atomic steps at the substrate surfaces. They are fabricated by inducing an inclination angle relative to the crystallographic plane during the cutting. In our experiment, we grow CoPt films on commercial-available vicinal Al2O3 (0001) substrates, which are schematically shown in Fig. 1(a). The CoPt films we grow exist an artificial composition gradient in the thickness direction, which are designed as the nominal multilayered structure of Pt(0.8)/Co(0.3)/Pt(0.6)/Co(0.5)/Pt(0.4)/Co(1) (thickness in nanometer). The vicinal angle of the substrates is denoted by \(\alpha\) (shown in Fig. 1(a)). In our study, we use substrates with different \(\alpha\)(\(\alpha\)= 0° 5°, 7°, 10°). If not specified, the vicinal substrate represent here denotes substrate with \(\alpha =7^\circ\), while \(\alpha =0^\circ\) for the flat substrate. We use the transmission electron microscopy (TEM) to characterize the cross-section of film structure, as shown in Fig. 1(b), a smooth and continuous film of ~ 6 nm in thickness is obtained. The composition of Co and Pt in the film structure was verified by energy dispersive spectrometer (EDS), as shown in Fig. 1(c). The line scanning of the EDS results marked by the yellow arrow in Fig. 1(b) revel that the Co and Pt elements exist an opposite composition gradient in the thickness direction, in accordance with our design of the film structure.
The crystal structure of the CoPt films could be verified by X-ray diffraction. Figure 1(d) show the \(2\theta\)line scan spectrums of the films deposited on flat (\(\alpha =0^\circ\)) and vicinal substrates (\(\alpha =7^\circ\)). For both samples we could observe a peak at 40.6°, this means that the CoPt films are (111) oriented, no matter the films are deposited on flat or vicinal substrates. The XRD peak also indicated that the multilayers have transformed to an alloying structure, due to the inter-diffusion. It should be noted that the Al2O3(0006)substrate peak is only observed in the flat substrate, this may be due to the larger surface roughness on vicinal substrates, due to the existence of additional atomic steps. We further performed the off-axis Phi-scan for two different samples, as shown in Fig. 1(e). For the CoPt grown on flat substrate, the Phi-scan pattern with CoPt (002) plane rotated along [111] axis show six-fold symmetry with each diffraction peak separated by 60°. For CoPt with cubic symmetry, one should only observe three-fold rotational symmetry if viewed along the [111] direction 21. The presence of the six diffraction peaks indicates that although it is (111) plane in z-direction, there is an additional type of twist domain in the material, where the domains are rotated along the substrate normal by 60°, similar with the situation when TiN (the same crystal structure type with CoPt) grown on Al2O3 (0001) substrates 25. While for the CoPt grown on vicinal substrate, the Phi-scan pattern changes into two-fold symmetry. The reduction of the rotation symmetry indicates that the in-plane symmetry of the CoPt film is broken when grown on vicinal substrate. The two-fold Phi-scan pattern indicated that crystal structure of the CoPt film probably evolve from cubic to monoclinic, due to the anisotropic lattice strain that are parallel and perpendicular with the atomic steps on the vicinal substrates.
Figure 1(f) shows the in-plane and out-of-plane magnetic hysteresis (M-H) loops for the CoPt layer deposited on vicinal substrate (\(\alpha =7^\circ\)). The results show that the in-plane and out-of-plane saturation fields are 1000 Oe and 190 Oe, respectively. The much larger in-plane saturation field and the square out-of-plane M-H loop indicate strong perpendicular magnetic anisotropy of the CoPt film. In supplementary information (SI) (Fig. S1), we further characterize the Ms and the perpendicular anisotropy Hk as a function of \(\alpha\). The results reveal that for the films deposited on vicinal substrates, the additional strain from the substrates only slightly influence the value of Ms and Hk.
Full scale field-free switching
Figure 2: Current-induced switching of the CoPt layer. (a) Schematic drawing of the experiment set up. (b) SOT switching of the CoPt films grown on the flat substrate (\(\alpha =0^\circ\)), measured at Hx = ± 100 Oe and 0 Oe. (c) SOT switching of the CoPt films grown on the vicinal substrate (\(\alpha =7^\circ\)). (d) Kerr images of the field-free switching process of the CoPt magnetization, for the films grown on vicinal substrates (\(\alpha =7^\circ\)). The bright domains and dark domains correspond to the up-ward and downward magnetization states, respectively. (e) Current and field (Hz) induced RH loops. Current-induced RH are measured with Hx = 0 Oe. (f) Field-free switching stability of the CoPt layer. Positive (+ 25mA) and negative (-25mA) current pulses are alternatively applied, the RH do not decay after ~ 300 switching cycles. (g) Switching ratio as a function of Hx, for CoPt films grown on substrates with different \(\alpha\). Inset of (g) shows Heff (denoted by the pink arrows) as a function of \(\alpha\).
Next, we characterize the SOT switching of the CoPt layer. The CoPt films grown on different substrates are patterned into Hall bar structures with 5 µm in width and 20 µm in length. Figure 2 (a) is the schematical drawing of the experiment set-up. Pulse currents (Ipulse) with a fixed duration (30µs) are applied along X-direction. After each pulse, the magnetization states are electrically read out by the anomalous Hall resistance (\({R_H}={V_{ac}}/{I_{ac}}\), RH∝Mz). The magnetization states could also be imaged by polar Kerr microscopy, which sensitive to the out-of-plane magnetization component. In-plane fields with different amplitudes Hx are applied along the current direction, to help the deterministic switching of the magnetization. Figure 2(b) shows the current induced switching of the CoPt layer that are grown on flat substrates. When the current pulses with different amplitudes are scanned, clear RH loops could be observed in the existence of Hx, but no loops when Hx = 0 Oe. The switching polarity are reversed with the direction of Hx. Such switching characteristics are in consistence with the typical SOT induced switching of the perpendicular magnetization 8,26, 15, indicating the SOT origin of the CoPt switching. The results also demonstrated that the field-free switching could not be realized for the CoPt film deposited on flat substrate. Figure 2(c) shows the switching behavior of the CoPt film grown on vicinal substrate (\(\alpha =7^\circ\)). As shown in Fig. 2(c), we also observe the reversal of switching polarity with the direction of Hx, indicating the same origin of the switching as that grown on flat substrates. The surprised results show that clear switching loops could be observed even in the absence of Hx, the critical Hx for the reversal of the switching polarity shift to 140 Oe. The comparison of the switching performance demonstrating the field-free switching of the CoPt layer is induced by vicinal substrate. The field-free switching process could also be directly imaged by Kerr microscopy. As shown in Fig. 2(d), when the current reach + 19 mA, the contrast of the Kerr image starts to change, indicating the switching of the magnetization, the critical switching current is in accordance with the current induced RH loop. Magnetic domains with reversed magnetization are first nucleated in the Hall bar, and then expand continuously through domain wall propagation with the increasing of the pulse current. The magnetization was fully switched at + 25 mA. It should be noted that when grown on vicinal substrate, the Kerr images reveal that the field-free switching of the CoPt is full-scale (100% switching ratio), which have not been realized previously. The switching ratio could be verified by current induced Hall resistance (\(\Delta {R_H}\)). As shown in Fig. 2(e), in the absence of the field, the current induced (\(\Delta {R_H}\)) is about \(2.15\,\Omega\), which are nearly the same with the field induced maximum change of the RH (\(\Delta R_{H}^{{\hbox{max} }}=2.20\Omega\)), demonstrating the switching of the CoPt magnetization is full-scale. We found that such field-free switching could only be realized when the current is perpendicular with the vicinal direction of the substrate (Y-axis in Fig. 2(a)), but could not when they are parallel, show in the SI (Fig. S2). We further test the switching endurance of our devices, we alternatively apply positive and negative current pulse with fixed amplitude (25 mA), which drive the CoPt switch back and forth continuously. As shown in Fig. 2(f), after ~ 300 cycles of switching, the Hall resistances at two different states exhibit negligible decay, demonstrating the high endurance of our system. Such high switching endurance also distinguish itself by using additional layers, such as antiferromagnetic layer or in-plane magnetic layers, where the magnetic structure are easily disrupted and result in the decay of the switching ratio [26].
We systematically characterize the switching behavior for devices grown on different vicinal substrates. We plot the switching ratio (defined as \(\Delta {R_H}/\Delta R_{H}^{{\hbox{max} }} \times 100\%\)) as a function of Hx, for films grown on different substrates (with different \(\alpha\)). The results are summarized in Fig. 2(g). Here the negative switching ratio denotes the opposite switching polarity. For the films deposited on flat substrate (\(\alpha =0^\circ\)), the curve is antisymmetric and we have\({R_H}({H_x})= - {R_H}( - {H_x})\). The switching ratio increase with the external field and reach 100% when \(|{H_x}|>100\,Oe\). For all the samples grown on different vicinal substrates (\(\alpha >0^\circ\)), at zero field the switching ratio could reach nearly 100%, demonstrating the wide operation window for such full-scale field-free switching. The critical field for zero switching shift from Hx = 0 Oe to nonzero values, which vary between 100 ~ 200 Oe, and is summarized in the inset of Fig. 2(g). These shift values reflect the effective in-plane field (Heff) the vicinal substrates could produce, and is critical for the realization of the field-free switching. As summarized in Table. 1, the Heff are much larger than that produced by other strategies, which ensure the high switching ratio compared with other strategies.
Quantitative Verification of the tilted anisotropy and DMI
Next, we explore the physical origin of the field-free switching. According to previous results, both the tilted magnetic anisotropy27 and Dzyaloshinskii–Moriya interaction (DMI) would play a critical role in the SOT the switching 17,28. For this reason, we quantitatively characterize these quantities. When the CoPt grown on the vicinal substrates, the stray fields between adjacent atomic steps and the uniaxial strain could induce the magnetic easy-axis (EA) tilt from normal of the film plane. Such tilted EA could be verified by analyzing the rotation of the magnetization with respect to the film planes. In Fig. 3(a)-(c), for the SOT device grown on the vicinal substrate (the sample in Fig. 2(c)), we characterize the field and angular dependence of the RH, by applying a current (1 mA) in the X-direction and measuring the RH along the Y-direction. Figure 3(a) show the field dependence of the RH when fields are scanned along X and Y directions. The field dependence of the RH curves along X and Y direction exhibits observable difference. The different RH curves along X and Y direction indicates that the EA is tilted from the normal direction of the film plane, or else the switching behaviors along different in-plane directions should be identical. To confirm the exact tilting plane, we further measure the angular dependence of the RH curves in the XZ and YZ plane. Figure 3(b) shows the angular dependence of the RH curves when fields with fixed amplitude (1 T) are rotated in two different planes. The angular dependence of the RH along the XZ and YZ plane exhibits distinguishable difference. The RH curve is symmetric about Z-axis (\({\theta _{xz}}={180^ \circ }\)) when rotated in the XZ plane, while asymmetric about Z-axis (\({\theta _{yz}}={180^ \circ }\)) when rotated in the YZ plane. As the rotation of the magnetization should be symmetric bout the EA, the symmetric and asymmetric rotational symmetry about the film normal (Z-axis) demonstrate that the magnetization is tilted in the YZ plane (along the atomic steps of the substrates). Such tilted anisotropy induced field and angular dependence of the magnetization switching behavior could be reproduced by the micromagnetic simulation (shown in the SI, Fig. S4). For comparison, we also measure the sample that are grown on flat substrate (shown in the SI, Fig. S3). The results reveal that the field and angular dependence of RH along different directions are identical, in contrast with the sample grown on vicinal substrate. From the above discussion, we could conclude that when grown on vicinal substrates, the anisotropy of CoPt would tilt along the atomic steps of the substrates (Y- axis).
The exact tilting angle of the EA (defined as \({\theta _{EA}}\)) could further be characterized by using the magnetic torquemetry 29. In a system with uniaxial anisotropy (Ku), when a strong enough magnetic field H is applied, energy density (E/V) could be expressed as:
$$E/V= - {M_s}H\cos (\theta - {\phi ^M})+{K_u}{\sin ^2}({\phi ^M})$$
1
where \(\theta\) is the angle between the applied magnetic field and the Z-axis, \({\phi ^M}\)is the angle between the magnetization and the Z-axis, and could be obtained by the RH measurement (\({\phi ^M}=\arccos ({R_H}/R_{H}^{{\hbox{max} }})\)). The equilibrium angle of the magnetization can be obtained by minimizing energy density with respect to \({\phi ^M}\):
$$l({\phi ^M})=H\sin (\theta - {\phi ^M})=({K_u}/{M_s})\sin 2({\phi ^M})$$
2
According to Eq. (2), the direction of EA corresponding to the direction where \(l({\phi ^M})=0\). As shown in Fig. 3(c), for the CoPt grown on the vicinal substrate, we measure the \(l({\phi ^M})\) as a function of \({\phi ^M}\) when the field (1 T) are rotated in the XZ and YZ planes. The results reveal there exists a phase difference for \(l({\phi ^M})\) measured in the XZ and YZ planes. When the field is rotated in the XZ plane, we have \(l=0\) when magnetization is along Z-axis (\(\phi _{{xz}}^{M}={180^ \circ }\)), indicating that the EA is parallel the Z-axis in the XZ plane. However, in the YZ plane, the torque curve exist a 10° phase shift compared with that in the XZ plane, with \(l=0\) when \(\phi _{{yz}}^{M}={190^ \circ }\), this reflect that the EA tilt 10° from Z-axis in the YZ plane when grown on vicinal substrate. In the SI (Fig. S3), we also measure the \(l({\phi ^M})\)for the sample grown on flat substrate, the results shown that there do not exist such phase difference for \(l({\phi ^M})\) in XZ and YZ planes, and we have \(l=0\) when \({\phi ^M}={180^ \circ }\), demonstrating that EA is not tilted when grown on flat substrate. We also characterize the \({\theta _{EA}}\) for films grown on different substrates, as shown in Fig. 3(d). The results reveal that the tilting of EA is universal when grown on vicinal substrates.
Next, we further characterize the DMI of our CoPt layers, using a method proposed by Kim et al, which is based on the magnetic droplet nucleation model 30. As depicted in the inset of Fig. 3(e), the hysteresis loop was measured by sweeping the magnetic field at an angle \(\theta\) with respect to the z-axis. With the increasement of \(\theta\), the switching field (Hsw) starts to decrease when \(\theta\) reach certain critical value, as shown in Fig. 3(e). If we denote the magnetic field where the magnetization is switched from the “down” state to the “up” state by Hsw, then the coercive field Hc and the accompanying in-plane field Hn can be expressed by \({H_{sw}}\cos \theta\) and \({H_{sw}}\sin \theta\), respectively. Figure 3(f) shows the measured Hc as a function of Hn. As described in earlier works, the curve shows a clear plateau, and Hc starts to decrease after Hn passes a threshold value, which corresponds to HDMI31. By using this manner, we characterize the HDMI for films grown on different substrates. The results are shown in Fig. 3(f). For CoPt grown on flat substrate, HDMI is ~ 230 Oe, in consistence with the pervious results 15,32. Our results also show a monotonously increasement of HDMI with \(\alpha\), and reach ~ 390 Oe when \(\alpha =10^\circ\). As previous results have shown that the strain from substrates would contribute a non-negligible DMI 33,34. Our result further demonstrate that the additional strain induced by the periodic atomic steps on the vicinal substrates could tune and enhance the DMI strength.
Simulation of the field-free switching
After characterizing the tilted anisotropy and DMI of our devices, we further verify the physical origin of the measured field-free switching, by using micromagnetic simulation. We consider the influence of the tilted anisotropy and DMI on the SOT induced magnetization switching. The simulation details are shown in the SI. We simulate the switching of a CoPt with\(200{\kern 1pt} {\kern 1pt} nm \times 50\,nm{\kern 1pt} {\kern 1pt} \times {\kern 1pt} {\kern 1pt} 4{\kern 1pt} \,nm\,(x \times y \times z)\) in size. We apply pulse currents with different amplitudes along X-direction, and record the magnetization states (Mz) after each pulse. The detail current sequences are shown in Fig. 4(a). External fields Hx with different directions are applied along the current direction, to help the deterministic switching. Figure 4(b) shows the switching of the CoPt layer with tilted anisotropy, with EA tilt toward different directions. When the EA is tilted along Y-axis (perpendicular with the current), clear switching loops could also be observed even at zero field, demonstrating the realization of the field-free switching in such switching geometry. While the EA is tilted along X-direction (parallel with the current), field-free switching could not be realized. Such switching behavior is in accordance with the experimental results in the SI (Fig. S2). Figure 4(c) shows the detail switching process, a domain with reversed magnetization was first nucleated and then expanded towards the edge by domain wall motion, until the entire domain was reversed. Such domain nucleation and domain wall motion process are in accordance with the Kerr images in Fig. 2(d). Besides, we also simulated the effects of DMI on the field-free switching. Figure 4(d) shows the influence of DMI on the SOT switching, in a CoPt layer with tilted anisotropy. The results reveal that the critical switching current decreasing and the increasement of DMI strength. This is because the DMI could inducing in-plane magnetization component at the edge of the hall bar structures. In CoPt system with perpendicular anisotropy, no matter with or without DMI (interface DMI, \(0.5mJ/{m^2}\)), field-free switching also could not be realized, excluding the possibility of DMI induced field-free switching (shown in SI (Fig. S5)). The above discussion demonstrates that tilted anisotropy is the origin of the field-free switching, while DMI could help decreasing the critical switching current. Previous results also have shown that vicinal substrate could tilt the anisotropy of L10-FePt, and induce the field-free switching 27,35.
Quantitative evaluation of the SOT effective field
We further quantitively characterize the SOT effective field and the SOT efficiency in our CoPt system, by using harmonic Hall voltage analysis. The measurement set up are schematically shown in the inset of Fig. 5(a), while an in-plane external magnetic field is swept (X-direction, with a small tilting angle 4° to the film plane), we measure the first (\({V_\omega }\)) and second harmonic Hall voltages (\({V_{2\omega }}\)) under an alternating (AC) current (\(\omega =13.7Hz\)) along X-direction. The second harmonic signal \({V_{2\omega }}\) is induced by the AC current, which exerts a periodic effective field on the magnetization. According to the harmonic analysis theory 36,37, the damping-like SOT effective field (HDL), which is the main origin of the SOT switching, could be evaluated from fitting the field dependent\(R_{{xy}}^{\omega }={V_{2\omega }}/{I_{ac}}\) data using the following equation:
$$R_{H}^{{2\omega }}=\frac{{{R_H}}}{2}\frac{{{H_{DL}}}}{{|{H_x}| - H_{k}^{{eff}}}}+{R_{offset}}$$
3
where RH is the anomalous Hall resistance, HDL and Roffset are the damping-like SOT effective field and resistance offset, respectively. (The field-like SOT effective field, which is much weak than HDL, could be evaluated when the fields are scanned along Y-direction (shown in Fig. S6 of SI). Figure 5(a) (b) plot the field dependence of \({V_\omega }\) and \({V_{2\omega }}\) signals for the CoPt grown on the vicinal substrate (\(\alpha =7^\circ\)), measured under different Iac (2, 3, 4, and 5mA), from which HDL could be calculated according to Eq. 3. We did not consider the influence of planner hall effects, for its influence on the \(R_{{xy}}^{{2\omega }}\) is negligible 15.As shown in Fig. 5(c), HDL exhibit a linear dependence with the amplitude of AC current, demonstrating the current origin of HDL. we further characterize the HDL for the CoPt deposited on different vicinal substrates (\(\alpha\)= 0° 5°, 7°, 10°). For all the samples, HDL exist distinguishable difference for the samples grown on different substrates, indicating the influence of the substrates on the HDL. To quantify such difference, we further calculate the SOT efficiency (\({\beta _{DL}}\)) and spin Hall angle (\({\theta _{SH}}\)) for the different samples. The SOT efficiency is defined as \({\beta _{DL}}={H_{DL}}/{j_{CoPt}}\), which could be obtained by fitting the current dependence of the HDL in Fig. 5(c). The spin Hall angle could also be calculated as:
\({\theta _{SH}}=\left( {\frac{{2e}}{\hbar }} \right){\mu _0}{M_s}{t_{FM}}{\beta _{DL}}\)
where e, \(\hbar\) and \({\mu _0}\) are the elementary charge, reduced Planck constant and permeability of vacuum, respectively. MS and tFM are the saturation magnetization and thickness of the CoPt films. Figure 5(d) show the \({\beta _{DL}}\) and \({\theta _{SH}}\) for films deposited on different vicinal substrates. For the films deposited on the flat substrate (\(\alpha =0^\circ\)), the calculated \({\beta _{DL}}\)= 3.1 Oe per 107 A/cm2, \({\theta _{SH}}\)= 0.008. For the devices fabricated on vicinal substrates (\(\alpha\)= 5°, 7°, 10°), our results show that the \({\beta _{DL}}\) and \({\theta _{SH}}\) have an enhanced of ~ 25%, compared with that grown on flat substrates. Thus, our results demonstrate that the vicinal substrate could not only induce field-free switching, but also increase the SOT efficiency. The tuning of the bulk SOT by vicinal substrate have also been observed in the L10-FePt system 27. This could be contributed to the strain effects, the strain induced by the additional atomic steps would change crystal symmetry and the modify the spin–orbit coupling, and orbital polarization 38.