Figure 2a shows the dc voltage as a function magnetic field H that measured at excitation frequency of 3GHz for sample Py/Cu(7nm)/Bi2Se3. The results for other frequencies can be found in Figure S2. The voltage signals consisting of symmetric (Vs) and antisymmetric (Vas) parts, which can be isolated by fitting the measured voltage (data curve) with the form
Here Hr is the FMR resonant field and ΔH is the line width of the signal. Vs is attributed to the injected spin current whereas Vas originated from anisotropic magnetoresistance (AMR) or anomalous Hall effect (AHE). Similar fitting is also done for other samples and Vs is extracted as shown in Figure 2b. It was found that Vs is larger in the presence of Cu layer. FMR experiments were also conducted as shown in Figures 2c and 2d. Figure 2d presents the frequency dependence of FMR line width for samples with different Cu thickness. The linear fitted slope is larger for bilayer and trilayer samples (Cu0, Cu3 and Cu7 denote tCu=0, 3, 7nm respectively) in comparison to single Py, indicating spin current injected into Bi2Se3, resulting in the broadening of the FMR line width and thus larger damping constant a. Interestingly, the aPy/Cu/TI was found decreases from 0.01262 to 0.01185 when increasing the thickness of Cu layer up to 7nm.
The resistance of the multilayer samples Rd were measured using four probe method. Jc is determined as Jc= Ic/w = Vs/wRd, where w and Ic are the width of the sample and charge current as shown in Figure 3a. We used the standard analysis of spin pumping on TI5,6,7 to evaluate the spin-to-charge conversion Jc/Js. Spin mixing conductance Geff¯ which is used to illustrate the efficiency of generating spin current is extracted using Equation (1):
where Ms is saturation magnetization of Py, tPy is thickness of Py and g is Landé factor and uB is the Bohr magneton. Ms is calculated using Kittel formula from f vs. Hr (Figure 2c). Da = aPy/Cu/TI - aPy and is determined by analysing DHpp vs. f as shown in Figure 2d. For the spin current densities that injected across the interface due to spin pumping, Equation (2) is utilized as shown below:
in which g is gyromagnetic ratio, w(=2pf) and hrf are frequency and amplitude of microwave magnetic field respectively. The calculated Js is presented in Figure 3b. By dividing Jc with Js, spin-to-charge conversion efficiency Jc/Js can be determined as shown in Figure 3c.
Figure 3a plots the Jc against tCu. There is an optimized Jc at thickness of 3 and 7nm. In contrast, Js is reduced when 3 and 7nm Cu were incorporated. The trend of Js vs tCu is consistent with the changes of aPy/Cu/TI, where effective damping constant is found decreases when 3 and 7nm Cu were introduced. Interestingly, a maximized Jc/Js is observed at tCu=7nm, where Jc/Js reaches ~2.7nm. This result suggests that the optimization of Jc/Js could be related to the decrease of Js due to the Cu insertion. To investigate the possible reason for the Jc/Js enhancement, we plot Jc/Js as a function of effective spin mixing conductance Geff¯ as shown in Figure 4a. Various Geff¯ values were obtained by changing the Cu layer thickness. Large Jc/Js is obtained at low value of Geff¯ (and thus minimum Js as shown in Figure 3b). We further examined the Jc vs. Geff¯ as shown in Figure 4b. There is no enhancement of Jc with increasing Geff¯, revealing the spin-to-charge mechanism may not be dominated by the bulk spin hall effect (SHE).14 Hence, we here suggest that the spin-to-charge conversion in our Py/Cu/TI system arises from inverse Edelstein effect, where the origin is the spin-momentum locked surface states of TI layer, same interpretation as other literatures.5,11
Low Geff¯ indicates strong spin backflow and spin memory loss (spin absorption) at the high SOC interface.16,17 Both factors are relevant in this Py/Cu/TI trilayer system. If we examine Geff¯ (Py/Cu/TI) at various tCu, as presented in Figure 4c, except for Py/Cu(3nm)/TI and Py/Cu(7nm)/TI, samples Py/TI, Py/Cu(9nm)/TI and Py/Cu(11nm)/TI exhibit Geff¯~1.25´1019 m-2, which is the typical value for metal-metal interfaces.18,19 As reported by Du et al., the effective spin mixing conductance of trilayer system (FM/Cu/NM, FM denotes ferromagnetic while NM denotes nonmagnetic material) is determined by the serial contribution of the two interfaces (FM/Cu and Cu/NM) and the spin resistance of Cu.13 Here we refer FM to Py while NM to TI film. One of the reason for the lower Geff¯ compared with GPy/TI¯ may be resulted from smaller spin conductance gCu/TI of Cu/TI than that of GPy/TI¯, similar to the case in Cu/Pt.13,14 However, since Geff¯ » GPy/TI¯ at tCu ³9nm, here we assume Cu/TI and Py/Cu present similar quality with GPy/Cu¯ » gCu/TI. Thus, by assuming degree of spin absorption at Cu/TI interfaces are similar in all cases, we suggest that the reason for lower Geff¯ of 3nm and 7nm Cu-based trilayer samples could be due to the strong spin accumulation at this ultrathin regime.13 Stronger spin backflow occurs, as compared to tCu³9nm, which eventually leads to reduction of Geff¯.
The decrease of Geff¯ seems have strong correlation to the spin-to-charge conversion efficiency. The next question is how such condition could increase the Jc/Js? Here we defined Jc/Js as lIEE = nft where nf is Fermi velocity of TI surface states and t is IEE relaxation time. As shown in the Figure 4d, t is modified due to the tunnelling current into TI, which is determined by momentum relaxation time tp and interface tunnelling time tt as shown in Equation (3):20
where lmf = nf tp = mean free path TI. According to this model, we proposed that the monotonic increase of lIEE with decreasing Geff¯ attributed to the modification of IEE relaxation time t due to additional tunnelling barrier (Cu) that limits the interface transmission rate (1/tt).20,21 lIEE is always lower than lmf due to the correction factor of (1+2tp/tt). It becomes clear that one can increase lIEE by reducing 1/tt, which can be done by introducing tunnelling barrier in between Py and TI layer. Using lIEE (tCu=7nm) =2.7nm and based on our previous ARPES result, nf =5.7´105 m/s,22 we find t~4.7fs, which is same order of magnitude as Bi/Ag23 and a-Sn/Ag6 interfaces. Our extracted lIEE(=2.7nm) is higher than 0.1-0.4nm in Bi/Ag Rashba interface,23 2.1nm and 2nm in TI SS of a-Sn/Ag6 and HgTe/HgCdTe7 respectively. We attribute the enhancement to the insertion of Cu tunnelling barrier. Although more theoretical calculation might be needed, our works indicate the importance of interface engineering to enhance the spin-to-charge conversion. This method could also be applied to other high SOC interfaces for obtaining high spin-to-charge conversion based on the inverse Edelstein effect, which is essential for spin current detector and other novel application such as broadband terahertz emitter.24,25