Supplementary Material Determination of intrinsic spin Hall angle in Pt Yi Wang, Praveen Deorani, Xuepeng Qiu, Jae Hyun Kwon, and Hyunsoo Yang Department of Electrical and Computer Engineering, National University of Singapore, 117576, Singapore S1- Analysis of the symmetric part in ST-FMR signals We carried out the microwave-network analysis measurement to calibrate the RF current (Irf) in our samples by a Vector Network Analyzer (VNA, Agilent PNX-X Network Analyzer, N5245A). The calibration schematic diagram is presented in Fig. S1. We connected two same length RF cables, two nominally same Bias-Tees, and two GSG probes and make GSG probes contacted on a “through” on a standard calibration kit. Here we assume each half of the circuit is the same and no power loss or reflection in the “through”. Hence, we identified the power loss in the Bias-Tee, 1 meter long RF cable, and GSG probe during the transmission by moving the calibration surface outside the measured circuit (denoted by the black dashed line). From the measured S11 and S21 parameters, the total power loss in the cables and connectors in our ST-FMR measurement was found to be 75% of the total input power. Thus, using 25% of power (13 dBm = 19.95 mW) in the equation P I rf 2 Z m 2 , we can calculate the Irf in different Pt (6 nm)/Ni81Fe19 (Py, 2 ‒ 10 nm) devices, respectively. We then used the following equations [S1] to obtain the spin Hall angle from the symmetric part of ST-FMR signal separately, Sym(Vmix ) I rf cos H dR 0 1 0 M st /E , and m s / ST Fsym (H ext ) , s J s /E ST 4 d H where Sym (Vmix) is the symmetric component of the ST-FMR signal, Irf is the RF 1 current flowing through the device, R is the anisotropic magnetoresistance as a function of angle between Irf and magnetic field Hext, is the linewidth of 0 ST-FMR signal, Fsym (Hext) is a symmetric Lorentzian, ST is the spin torque on unit Ni81Fe19 (Py) moment by spin currents at H = 0o, s is the spin Hall conductivity, is the conductivity, t is the thickness of Py, E is the microwave field, and m is the measured spin Hall angle, respectively. Vector Network Analyzer (VNA) Calibration Surface Bias-Tee Bias-Tee RF cable GSG probe “Through” on calibration kit Figure S1: The calibration schematic diagram to calibrate the RF current (Irf) in our samples by a Vector Network Analyzer (VNA). We have plotted together the Py thickness dependent spin Hall angle from both methods (by taking the ratio of the symmetric (S) and antisymmetric components (A) of the ST-FMR signals, and separate calibration) in Fig. S2. The error bars are from the slight uncertainty of the measurement angle in dR /d H . We find that there is not a significant difference between the results from the two measurement techniques. Results from both methods show that the measured spin Hall angle increases as the Py thickness increases in thin Py thickness range. This confirms that the thickness dependent spin Hall angle does not originate from the in-plane effective-field component of current-induced spin torque when the Py layer is thin. 2 Ratio S/A T = 300 K Separate calibration 0.12 m 0.09 0.06 0.03 0 2 4 6 tNiFe (nm) 8 10 Figure S2: The Py thickness dependent spin Hall angle obtained by taking the ratio of the symmetric (S) and antisymmetric components (A) of the ST-FMR signals, and separate calibration method only by symmetric components (S). S2- The magnetic field angle for the largest ST-FMR signals The Vmix spin torque ferromagnetic resonance (ST-FMR) signal is dR cos ( H ) , where H is the angle between the magnetic field and applied d H RF current Irf [S2]. The resistance of the Pt/Py microstrip can be written as R R0 R cos 2 ( H ) due to the anisotropic magnetoresistance (AMR) effect. Consequently, dR 2R sin ( H ) cos ( H ) sin ( H ) cos ( H ) [maximum value is d H occurred at H = 45o], and Vmix cos 2 ( H ) sin ( H ) [maximum value is achieved at H ~ 35]. Thus, although the change of AMR is maximum at H = 45, the largest ST-FMR signals is achieved at H ~ 35. S3- Possible sources of measurement artifact Heating effect due to input RF Power (P) Figure S3(a) shows the measured ST-FMR signals on Pt (6 nm)/Py (5 nm) device at a nominal input RF power (P) spanning from 9 to 16 dBm (i.e. 7.95 – 39.8 mW ) at f = 8 GHz and T = 300 K. The extracted peaks of ST-FMR signals (open symbols) as 3 a function of P are plotted in Fig. S3(b) with a linear fit (solid line). From this observation, we find that the response of our device is in the linear regime up to P = 16 dBm (39.8 mW). As shown in Fig. S3(c), the measured spin Hall angle m remains constant as a function of P at T = 300 K. This indicates that there is no significant heating effect in our ST-FMR measurements. Device impedance (Zm) As shown in Fig. S3(d), we confirm that m determined from a Pt (6 nm)/Py (5 nm) device is independent of device impedances (Zm) ranging from 33 to 60 Ω at f = 8 GHz, with an input RF power P = 13 dBm and T = 300 K. 50 (a) 9 dBm 10 dBm 11 dBm 12 dBm 13 dBm T = 300 K f = 8 GHz 0 -50 90 Vmix (V) Vmix (V) 100 14 dBm 15 dBm 16 dBm 500 1000 1500 (b) 60 30 0 10 Hext (Oe) (c) 20 30 40 P (mW) T = 300 K f = 8 GHz 0.09 m m 0.09 Data Fitting 0.06 (d) T = 300 K f = 8 GHz 0.06 0.03 0.03 9 10 11 12 13 14 15 32 16 36 40 44 48 52 56 60 Zm () P (dBm) Figure S3: (a) The measured ST-FMR signals on a Pt (6 nm)/Py (5 nm) device at different nominal input RF power P (dBm) at f = 8 GHz and 300 K. (b) The extracted peaks of ST-FMR signals (open symbols) as a function of P (mW) with a fit (solid line). (c) Measured spin Hall angle m determined from a Pt (6 nm)/Py (5 nm) device as a function of P. (d) m as a function of impedance Zm at f = 8 GHz. The red dashed lines are guides to the eye. 4 Magnetic field component (Hem) of electromagnetic wave As shown in Fig. S4(a), in addition to the RF-current induced Oersted field (Hrf) and spin current Js, the Oersted field (Hem) due to RF signals transmitting along the coplanar waveguide (CPW) may exist and exert torque ( m̂ H em ) on the Py layer. The out-of-plane component of Hem also yields symmetric Lorentzian peaks with the same signals for both directions of Hext [S3, S4], which could lead to a slight overestimation or underestimation of S/A depending on the Hext direction, and thus the spin Hall angle sh . In our work, as shown in Fig. S4(b), the effect caused by Hem was eliminated by locating the microwave GSG probe at a proper position around the center of CPW, yielding the same amplitude of S/A and sh with both directions of Hext. Furthermore, we have made a control ST-FMR device Pt (6 nm)/Py (5 nm) with symmetric CPW as shown in Fig. S4(c). The measured spin Hall angle is ~ 0.063 at 8 GHz and room temperature. This value is consistent with what we obtained in our manuscript (0.063) by using the Pt (6 nm)/Py (5 nm) device as shown in Fig. 3S(b). z (a) x W y Hem Jc Js L Pt NiFe Hrf Pt/Py strip (b) (c) ST-FMR device G S G GSG Probe G S G Figure S4: (a) The Pt/Py microstrip with the charge current Jc, spin current Js, RF Oersted field (Hrf), and the Oersted field (Hem) due to RF signals transmitting along the coplanar waveguide (CPW). (b) The layout of CPW for the ST-FMR devices used in our ST-FMR measurements. (c) The layout of the CPW for the control ST-FMR device. 5 S4- Meff vs. Ms at different Py thicknesses As shown in Fig. S5(a), the 4πMeff (from the Kittel fitting) decreases dramatically as the Py thickness decreases from 10 to 2 nm. The saturation magnetization Ms of Py at different thicknesses were independently measured by vibrating sample magnetometer (VSM). As shown in Fig. S5(b), it is found that there is a discrepancy (~33% for 2 nm Py and ~11.6 % for 3 nm Py) between Meff and measured Ms, which indicates a weak perpendicular anisotropy at the Pt/Py interface, calculated from 4 M eff 4 M s 2 Ks /(M st ) , where Ks is the perpendicular interface anisotropy, and t is the thickness of the Py layer. When t > 4 nm, the discrepancy almost disappears. 4Meff (T) 1.0 (a) 4Meff 0.8 T = 300 K 0.6 0.4 (Ms-Meff)/Ms (%) 30 (b) T = 300 K 20 10 0 1 2 3 4 5 6 tNiFe (nm) 7 8 9 10 Figure S5: The 4πMeff (a) and the difference (b) between Ms and Meff as a function of Py thickness at 300 K. S5- Damping constant eff for different Py thicknesses The linewidth (∆H) was extracted from the fitting of ST-FMR signal. Accordingly, the effective damping constant eff was determined by eff (H )/2 f [S2, S5] and was found to increase from 0.0123 (Py = 10 nm) to 0.063 ± 0.003 (Py = 2 nm), as seen in Fig. S6. This could be possibly attributed to the spin pumping effect [S6, S7], 6 film inhomogeneous broadening, and/or two-magnon scattering [S8]. Damping Constant 0.07 T = 300 K 0.06 0.05 0.04 0.03 0.02 0.01 1 2 3 4 5 6 7 tNiFe (nm) 8 9 10 Figure S6: The effective damping constant eff as a function of Py thickness at 300 K. S6- Estimation of spin pumping contributions in ST-FMR signals The possible existence of spin pumping contribution to the symmetric components of the ST-FMR signals might also cause the Py thickness dependent spin Hall angle. In order to clarify this and confirm our claim in the main text, we have estimated the spin pumping contribution for samples covering the full range of different Py thicknesses by the following equations [S1]. VSP m eW S R t eff tanh ( Pt )Re(g )P2 sin ( H ) H ext /(H ext 4 M eff ) , 2 2S P 1 2 dR /d H I rf S 2 A2 , where VSP is the spin pumping signal in our ST-FMR measurements, W is the microstrip width, R is the device resistance, λS is the spin diffusion length in Pt, m is eff the measured spin Hall angle, tPt is the Pt thickness, Re( g ) is the real part of the effective spin mixing conductance ( 2×1019 m-2), H is the angle between Irf and magnetic field Hext, Irf is the RF current flowing through the device, P is the maximum precession angle in the device plane, S and A are the symmetric and antisymmetric components of the ST-FMR signal, respectively. The estimated spin pumping contribution VSP together with S as a function of Py thickness are shown in Fig. S7. We have found that the estimated spin pumping signals for all the devices in 7 the full range of different Py thicknesses are extremely small (all less than 0.75 V) as compared to the measured symmetric component S (tens of V) in our ST-FMR measurements. The ratios of VSP/S are less than 4%. Hence, we confirm that the spin pumping contributions in our ST-FMR measurements are negligible and will not cause the Py thickness dependent spin Hall angle shown in Fig. 3(a) in the main text. 30 V (uV) 25 20 15 Measured S Estimated VSP 10 5 0 0 2 4 6 tNiFe (nm) 8 10 Figure S7: The estimated spin pumping contribution VSP together with symmetric component S as a function of Py thickness. References in Supplementary Material: [S1] A. R. Mellnik, J. S. Lee, A. Richardella, J. L. Grab, P. J. Mintun, M. H. Fischer, A. Vaezi, A. Manchon, E. A. Kim, N. Samarth, and D. C. Ralph, Nature 511, 449 (2014). [S2] L. Q. Liu, T. Moriyama, D. C. Ralph, and R. A. Buhrman, Phys. Rev. Lett. 106, 036601 (2011). [S3] M. V. Costache, S. M. Watts, M. Sladkov, C. H. van der Wal, and B. J. van Wees, Appl. Phys. Lett. 89, 232115 (2006). [S4] M. Harder, Z. X. Cao, Y. S. Gui, X. L. Fan, and C. M. Hu, Phys. Rev. B 84, 054423 (2011). [S5] C. F. Pai, L. Q. Liu, Y. Li, H. W. Tseng, D. C. Ralph, and R. A. Buhrman, Appl. Phys. Lett. 101, 122404 (2012). [S6] Y. Tserkovnyak, A. Brataas, and G. E. W. Bauer, Phys. Rev. Lett. 88, 117601 (2002). [S7] P. Deorani, and H. Yang, Appl. Phys. Lett. 103, 232408 (2013). [S8] X. Y. Liu, W. Z. Zhang, M. J. Carter, and G. Xiao, J. Appl. Phys. 110, 033910 (2011). 8