Bismuth (Bi) or Bi-based heterostructures has attracted much interest as candidates for spin current generator. Recently, helicity-dependent (HD) photocurrent in Bi or Bi/Cu(or Ag) thin films was reported by using pulse laser-induced terahertz (THz) emission and transport measurement[1, 2]. It is believed that spin current in Bi induced by circularly-polarized laser via photo-spin conversion effect is converted into charge current via spin-charge conversion effect. However, details of photo-spin conversion in Bi have yet to be clarified because the photo-spin and the spin-charge conversion effects are observed simultaneously, thus, one cannot distinguish two effects. Here, we studied THz emission induced by spin-current generation using the photo-spin conversion effect in Bi and the laser-induced demagnetization in an adjacent ferromagnetic Co layer in Bi/Co films to separate two spin-related conversion effects and investigate the photo-spin conversion in Bi.
The samples, glass sub./Bi(tBi)/Co(5)/MgO(2)/Ta(2) (thickness is in nm), were prepared by a DC/RF magnetron sputtering. Laser-induced THz emission in Bi/Co films was investigated by THz time-domain spectroscopy (THz-TDS) with 120-fs Ti: Sapphire laser[3,4]. Figure 1 and Figure 2 show the Bi thickness tBi dependence of THz peak values induced by linearly-polarized laser and HD-THz peak values, respectively. Here, HD-THz is difference between signals obtained with left- and right-circularly polarized laser. We found different tBi dependence as shown in Fig. 1 and Fig. 2, which is possibly due to the difference in spin-relaxation length of two experiments. In the presentation, we will discuss the physics behind the different THz signals obtained in two experiments and quantitative consideration of the photo-spin conversion in Bi. This work is partially supported by KAKENHI (19K15430, 21H05000). K. I. acknowledges Grant-in-Aid for JSPS Fellow (22J22178) and GP-Spin at Tohoku University. S. M. acknowledges CSRN in CSIS at Tohoku University. 
**References** [1] Y. Hirai et al. Phys. Rev. Appl. 14, 064015 (2020)
[2] H. Hirose et al. Phys. Rev. B 103, 174437 (2021)
[3] H. Idzuchi, et al., AIP Advances 11, 015321 (2021)
[4] Y. Sasaki et al. Appl. Phys. Lett. 111, 102401 (2017)
 
![](https://s3.eu-west-1.amazonaws.com/underline.prod/uploads/markdown_image/1/image/1c6b849cf1cb074f28ed75dea6cdba3d.png)

Laser induced terahertz wave emission from Bi/Co structure

All Optical Helicity Independent Switching (AO-HIS) of magnetization, using single femtosecond laser pulses, has been demonstrated in GdFeCo ferrimagnetic alloys for various concentrations [1] as well as in other structures with antiferromagnetic coupling, Gd/Co, [Tb/Co]n/Ta/CoFeB and Mn2RuxGa [2,3,4]. Up to now, AO-HIS has never been observed for ferromagnetic layers. However, it was shown that a single pulse magnetization reversal of a ferromagnet could be observed in a spin-valve structure [5]. The switching is then achieved by the ultrashort spin current pulse generated from the ultrafast demagnetization of GdFeCo [5,6]. In this work, we study Gdx(FeCo)1-x/Cu/FM spin-valve structures, where FM can be different ferromagnetic layers [7] and the composition x of the GdFeCo alloy is also changed [8]. By increasing the Gadolinium concentration x, we aim at increasing the spin current injected in the copper layer [6]. We show that this can reduce the laser fluence threshold required to observe the FM magnetization reversal. In particular, no AO-HIS of the GdFeCo layer is required and the threshold fluence for the FM layer is around 1.6 mJ/cm2 i.e. comparable to GdFeCo and Gd/Co multilayers [1,2] and smaller than what is achieved for Tb/Co/CoFeB [2] and Mn2RuxGa [3]. We also show that by changing the Curie temperature, the laser pulse duration and the Cu/FM interface, one can control the interaction between the spin current and the FM layer and so the laser fluence threshold. Finally, we measured the dynamics of the reversal of the FM layer, which happens in around a picosecond. We show a model, based on a recent theory for the ultrafast magnetization dynamics of ferromagnets [9], that explains this behavior. We thus designed spin-valve structures that could provide technological advantages regarding both speed and energy efficiency of data storage.

Ultrafast Single Pulse All Optical Magnetization Switching of Ferromagnets

An efficient electrical switching of thin film metallic nanomagnets has been demonstrated by using ferromagnet/heavy metal thin film heterostructures [1][2]. The spin-Hall effect in the heavy metal layer and/or the Rashba-Edelstein effect at the interface have been used to control the nanomagnets efficiently by electrical means. On the other hand, optically induced switching of nanomagnets might be useful for optically-switchable magnetic memories, promising candidate for future fast and low power consumption information processing system using photonic integrated circuits [3]. An increase of optical spin generation efficiency in the materials is crucial for such photo-spintronics devices. Recently, optical helicity induced torque on magnetization in metallic thin films [Fig. 1], termed as optical spin torque, has been reported. It was demonstrated that the optical spin torque is induced by the inverse Faraday effect in ferromagnetic metals and the optical orientation effect in nonmagnetic heavy metal layers [4][5]. Both the inverse Faraday effect and the optical orientation effect can be considered as bulk effects in the ferromagnetic layers and the heavy metal layers, respectively. However, interfacial nature of the optical spin generation such as the optical Rashba-Edelstein effect [6] has not been addressed so far. In this study, optical spin torque vectors in the ferromagnet/heavy metal heterostructure with different thicknesses and symmetry of stacking structures were investigated to gain insight into the interfacial nature of optical spin generation [7]. Thin film samples were fabricated by using magnetron sputtering technique. The stacking structure is as follows, Si/SiO2 sub./ MgO(10) / Fe50Co50 (dFeCo) / Pt (dPt) (thickness is in nm). FeCo (Pt) thickness dFeCo (dPt) was varied from 1 (2) nm to 4 (10) nm. To study the effect of symmetries for the stacking structure, samples with following stacking structure were also made, Si/SiO2 sub./ Pt(3) / Co(2) / Pt(3), Si/SiO2 sub./ Pt(3) / Co(2) / Ta(2), Si/SiO2 sub./ Co(2) / Pt(3). The optically induced spin was detected by using all-optical time-resolved magneto-optical Kerr effect (TRMOKE). The wavelength and pulse duration were 800 nm and 120 fs, respectively. The pump beam is irradiated on the film at an angle of 10 deg. measured from film normal. Polar MOKE signals were detected to measure normal component of magnetization. In-plane magnetic field up to 2 T was applied. Right circularly polarized (RCP) and left circularly polarized (LCP) pump pulses were irradiated on the ferromagnet/heavy metal heterostructure films. A change in the phase of magnetization precession was observed when the pump laser pulses with different optical helicities were irradiated, indicating the magnetization precession was excited by the optical spin torque. Figure 2 shows optical helicity induced TRMOKE signals where signals are obtained by taking differences between the signals with RCP and LCP pump pulses. Large peak at around delay zero is due to the so-called specular inverse Faraday effect, which is used to define the time when the pump pulse arrives at the film surface. Oscillation signals were fitted by the sinusoidal decayed function, as shown with broken curves in Fig. 2 bottom. The optical helicity induced TRMOKE signals were decomposed into sine and cosine components, as shown with red and blue solid curves in Fig. 2, respectively. This phase analysis was used to evaluate optical spin torque vectors in the heterostructures. The cosine signal indicates that magnetization precession is excited by out-of-plane optical spin torques, which can be explained by the optical orientation effect in the heavy metal Pt layer. In addition, remarkable sine signals was observed. The in-plane field-like optical spin torque evaluated from the sine signal was found to be increased with decreasing FeCo thickness. This increase cannot be explained by the inverse Faraday effect in the ferromagnetic FeCo layer [7]. A possible explanation is that the remarkable in-plane field-like optical spin torque is attributed to the interface spin generated by the optical Rashba-Edelstein effect. Interfacial in-plane torques can be induced by exchange coupling between generated spins and magnetization, which is analogous to the electrical manipulation of magnetization via the Rashiba-Edelstein effect. To validate the optical spin torque induced by the optical Rashba-Edelstein effect, we measured the optical spin torque with changing stacking structure symmetry. It was found that the in-plane optical spin torque was enhanced when Co was sandwiched by SiO2 and Pt layer, i.e., asymmetric heterostructure [7]. This result supports the optical spin torque induced by the interfacial Rashba spin-orbit coupling owing to the structural inversion symmetry breaking. In conclusion, we studied optical spin torque vectors in the ferromagnet/heavy metal heterostructure. By changing the thickness and the stacking structure symmetry of the heterostructure, we found new type of the interface optical spin generation, optical Rashba-Edelstein effect. This work will lead to efficient optical manipulation of thin film nanomagnets.

**References:**

[1] I. M. Miron, K. Garello, G. Gaudin et al., Nature, Vol. 475, p. 189 (2011) [2] L. Liu, C. -F. Pai, Y. Li et al., Science, Vol. 336, p. 555 (2012) [3] H. Becker, C. J. Krückel, D. V. Thourhout et al., IEEE J. Sel. Top. Quant., Vol. 26, p. 8300408 (2020) [4] G. -M. Choi, A. Schleife, D. G. Cahill, Nat. Commun. Vol. 8, p. 15085 (2017) [5] G. -M. Choi, J. H. Oh, D. -K. Lee et al., Nat. Commun. Vol. 11, p. 1482 (2020) [6] V. M. Edelstein, Phys. Rev. Lett. Vol. 80, p. 5766 (1998) [7] S. Iihama, K. Ishibashi, S. Mizukami, Nanophotonics, 20200571 (2020)

**Images:**

![](https://assets.underline.io/uploads/markdown_image/1/image/622c5ff6e97b66c2b5430e3384c20386.jpg)
Schematic illustration of the optical spin torque in a ferromagnet/heavy metal heterostructure.

![](https://assets.underline.io/uploads/markdown_image/1/image/466eff3367e9340d6519f6562b628362.jpg)
Optical helicity induced TRMOKE signal obtained by taking differences between signals with RCP and LCP pump pulses for a FeCo(2) / Pt(3) thin film. The optical helicity induced signals at around t = 0 [top] and magnetization precession due to the optical spin torque [bottom].

 Interface optical spin generation in a ferromagnet/heavy metal heterostructure

Synthetic antiferromagnets (SyAFs) are an excellent platform to explore novel spintronic and magnonic concepts with coupled magnetic moments[1,2]. Unlike a homogeneously magnetised single-layer ferromagnet, coupled magnetic layers are able to offer rich magnetic states where the competition between interlayer exchange coupling, external-field-induced Zeeman interaction as well as other magnetic anisotropy terms plays a role. This can expand into their dynamic regimes as the coupled moment nature inherently provides two eigenmodes, acoustic and optical modes[3-7], where time-dependent components of two coupled moments are oscillating in-phase (acoustic) and out-of-phase (optical)in a spin-flop (canted) regime. When we excite spin-waves by oscillating magnetic fields, the spatial symmetry/profile of microwave excitation determines which spin-wave modes are excited. In the simplest case, a uniform distribution of microwave excitation fields across a magnet can excite the uniform spin-wave mode (wavevector k = 0) as well as higher-order spin-wave resonance modes (k &gt; 0) with odd index numbers since the spatial profile of the microwave excitation and spin-wave mode amplitude (with phase) matches to each other in terms of symmetry. This in turn suggests that it should be possible to control the selection rules of spin-wave excitations by designing the spatial profile of excitation fields. Accessing hidden spin-wave states as well as tailoring spin-wave excitation efficiency by this approach has not been much explored in the past. We report in this work the current-induced-torque excitation of acoustic and optical modes in Ta/NiFe/Ru/NiFe/Ta synthetic antiferromagnet stacks grown on SiO2/Si substrates(Fig 1(a)). The two Ta layers serve as spin torque sources with the opposite polarisations both in spin currents and Oersted fields acting on their adjacent NiFe layers. This can create the odd symmetry of spatial spin torque distribution across the growth direction, allowing us to observe different spinwave excitation efficiency from synthetic antiferromagnets excited by homogeneous torques. We analyse the torque symmetry by in-plane angular dependence of symmetric and anti-symmetric lineshape amplitudes for their resonance (as shown in Fig 2(a-b)) and confirm that the parallel (perpendicular) pumping nature for the acoustic (optical) modes in our devices, which is in stark difference from the modes excited by spatially homogeneous torques. The terms parallel (perpendicular) pumping here signify that the torque (hence spin-wave excitation efficiency) is maximised when the oscillating fields and dc magnetic field are collinear(perpendicular) to each other respectively. This is evident from Fig 2(c-d) that strongly suggests the torque symmetry for the acoustic(optical) mode excitation being of form sin Φ(cos Φ) . We also generalize macrospin model for this particular spin-torque excitation geometry, which excellently supports our experimental observation. Our results offer capability of controlling spin-wave excitations by local spin-torque sources and we can explore further spin-wave control schemes based on this concept. We envisage that the control of spin-wave excitations in STT nanodevices will be useful for future spintronic and magnonic nano-devices.

**References:**

[1] R. A. Duine, K.-J. Lee, S. S. P. Parkin, and M. D. Stiles, Nat. Phys. 14, 217 (2018). [2] A. V. Chumak, V. I. Vasyuchka, A. A. Serga, and B. Hillebrands, Nat. Phys. 11, 453461 (2015). [3] F. Keffer and C. Kittel, Phys. Rev. 85, 329 (1952). [4] J. J. Krebs, P. Lubitz, A. Chaiken, and G. A. Prinz, J. Appl. Phys. 67, 5920 (1990). [5] S. M. Rezende, A. Azevedo, and R. L. Rodrguez-Surez, J. Appl. Phys. 126, 151101 (2019). [6] A. Sud, Y. Koike, S. Iihama, C. Zollitsch, S. Mizukami, H. Kurebayashi, arXiv:2012.12999 . [7] A. Sud, C. W. Zollitsch, A. Kamimaki, T. Dion, S. Khan, S. Iihama, S. Mizukami, and H. Kurebayashi, Phys. Rev. B 102, 100403(R) (2020).

**Images:**

![](https://assets.underline.io/uploads/markdown_image/1/image/b406e148e73969fbd07f012bcc683fa7.jpg)
FIG. 1: (a) A schematic of the sample geometry used for STT-FMR measurements in our study. (b) V obtained at different frequencies for acoustic and optical modes in our device for Φ = 55ο (the values for some frequencies have been scaled to show them properly). (c) A 2D colorplot of V as a function of applied field and frequency, measured for Φ = 55ο . (d) Numerical results calculated for the experimental conditions as in (c).

![](https://assets.underline.io/uploads/markdown_image/1/image/aaeaf82e3f75f0759e29b390a7923bff.jpg)
FIG. 2: (a-b) Angular dependence of symmetric (Vsym) and antisymmetric (Vasy) components of voltage for (a) acoustic mode measured at 8 GHz and (b) optical mode measured at 8.5 GHz. The solid curves are obtained using theoretical model. (c-d) The symmetry of torques obtained by dividing the Voltage by (c) sin 2Φ for acoustic mode and (d) cos 2Φ for optical mode. The dominant sin Φ (cos Φ) dependence of torques confirms the parallel(perpendicular) pumping configuration.

 Parity-controlled spin-wave excitations in synthetic antiferromagnets

Quantum magnonics is a rapidly growing field offering myriad of potential applications[1,2] particularly in the realm of coherent information processing. Magnons which are the collective excitations of spins offer exotic functionalities such as the ability to couple to various dynamic systems. Realisation of strong coupling , owing to large spin densities, which is tunable into the ultrastrong coupling regime makes them suitable for coherent information exchange at much faster speeds. Apart from this the easily accessible gigahertz frequency range, simple fabrication and miniaturization provides an ideal platform for incorporation in various microwave electronic circuits. Recently[3,4,5], Synthetic Antiferromagnets(SyAF) have attracted prodigious interest due to the controllable exchange coupling in the GHz regime making them a test bed for various magnonic applications[6]. Moreover, the substantially large mode volume overlapping gives them an advantage over light-matter interactions in attaining higher a coupling strength. A SyAF consists of two ferromagnetic thin films (FM) with an antiferromagnetic exchange coupling separated by a non-magnetic spacer (NM). When the two FMs are symmetric, a mode crossing occurs between symmetry protected in-phase and out- of -phase resonance precessions via in-plane external magnetic field tuning. This is reminiscent of degeneracy between even and odd parity magnons. This degeneracy and subsequent mode crossing can be lifted by breaking the symmetry either extrinsically or intrinsically. Extrinsic symmetry breaking (SB) can be exerted by tilting the external magnetic field out-of-plane which shifts the rotational symmetry axis from the SyAF plane, and the system is no longer symmetric under two-fold rotation. This leads to hybridization of the two modes and an anticrossing gap is generated. Additionally, a coupling gap can be induced by dynamic dipolar interaction[3]. The strength of the coupling between two magnon modes is determined by the size of the gap. Maximizing the coupling efficiency is thus easily attainable by the controllability of the coupling gap by external magnetic field orientation. Apart from an extrinsic control of coupling strength the symmetry of the system can be broken intrinsically by using either two different FMs or the same FMs with different thickness. This would lead to a coupling gap even for the external applied fields applied in-plane, owing to a change of magnetization under two-fold rotation. In this work we demonstrate the control of magnon-magnon coupling in SyAFs via intrinsic and extrinsic SB. The schematic of the two modes in SyAF system is shown in Fig 1(a). We first consider a symmetrical SyAF structure CoFeB/Ru/CoFeB as in Fig 2(a). The apparent mode crossing results from a degeneracy of two non-interacting modes which is protected by a two-fold rotational symmetry. By tilting the external field (see Fig 2(b)) we break this symmetry and an anticrossing gap appears. This demonstrates the extrinsic SB. When two FMs with different thickness are considered an inherent SB exists in the system which opens a gap even for an in-plane field as in Fig 2(c). Further, breaking the symmetry as in 2(d) by tilting the field leads to an increase of the gap and thus the coupling strength. This effect can be further enhanced when using two FMs of different materials, exhibiting a large coupling gap for an in-plane field as in Fig 2(e). Here, the coupling strength far exceeds the losses, described by the frequency half-width at half maximum of the individual modes. The absolute coupling strength reaches 30% of the mode frequencies, indicating the onset of the ultrastrong coupling regime. By calculating the coupling gap as a function of external field tilt angle we can putatively claim that both intrinsic and extrinsic SB can realise strong magnon-magnon coupling in SyAFs. Further, the strong coupling leads to an entanglement between even and odd parity modes, making it attractive for quantum information applications. We generalize a theoretical model in the macro spin limit by solving the two coupled LLG(Landau Lifshitz Gilbert) equations to describe the microwave absorption spectroscopy for the SB induced coupling in SyAFs. This study should shed light on the potential of SyAFs for studying and controlling magnon-magnon coherent coupling at room temperature. Moreover large tunable coupling strengths in this system will provide a novel platform for increased control of quantum systems.

**References:**

[1] G. Kurizki, P. Bertet, Y. Kubo, K. Mølmer, D. Petrosyan, P. Rabl, and J. Schmiedmayer, Proc. Natl. Acad. Sci. U.S.A. 112, 3866 (2015). [2] M. Ruggenthaler, N. Tancogne-Dejean, J. Flick, H. Appel, and A. Rubio, Nature Reviews Chemistry, 2(3), pp.1-16 (2018). [3] Y. Shiota, T. Taniguchi, M. Ishibashi, T. Moriyama, and Teruo Ono, Phys. Rev. Lett. 125, 017203 (2020). [4] A. Sud, C. W. Zollitsch, A. Kamimaki, T. Dion, S. Khan, S. Iihama, S. Mizukami, and H. Kurebayashi, Phys. Rev. B 102, 100403(R) (2020). [5] M. Ishibashi, Y. Shiota, T. Li, S. Funada, T. Moriyama, and T. Ono, Sci. Adv. 6, eaaz6931 (2020). [6] A. Guedes, M. J. Mendes, P. P. Freitas, and J. L. Martins, Journal of applied physics 99,08B703 (2006).

**Images:**

![](https://assets.underline.io/uploads/markdown_image/1/image/fda936d0116f14aa194f61f7d6f95187.jpg)
Fig 1. (a) Schematic of resonance modes in SyAFs. Two moments (m1 and m2) are coupled antiferromagnetically and canted at equilibrium. Under microwave irradiation, they precess in-phase (acoustic mode) and out-of-phase (optical mode) at different angular frequencies ωac and ωop respectively .We define θB as in the figure. (b) Schematics of the magnon-magnon coupling phenomena. When the exchange field (Bex) is small or two moments are within the film plane, the coupling strength (g) is zero and we can valve g by tuning Bex and θB.

![](https://assets.underline.io/uploads/markdown_image/1/image/7eaef5b95c81b3bc4450cc2312714f60.jpg)
Fig 2. Microwave transmission as a function of frequency.(a) For CoFeB(5)/Ru(0.5)/CoFeB(5) at θB = 90°, the two modes show mode crossing (b) At θB = 25° a gap appears. (c) In NiFe(5)/Ru(0.4)/NiFe(3) intrinsic SB occurs and the gap is seen for θB = 90° which increases as in (d) for θB = 30°. (e) CoFeB(3)/Ru(0.5)/NiFe(3) showing large gap at (e) θB = 90° and (f) θB = 20°. (g-h) Coupling strength g/2π as a function of θB which increases as the tilt angle is increased.* The numbers in brackets are the thickness of the FM layer in nm.

 Modulation of magnon-magnon coupling by inherent symmetry breaking in synthetic antiferromagnets

Manipulation of magnetization precession, namely magnon, with circularly-polarized light has attracted much attention. Many of relevant studies have focused on magnon driven by the inverse Faraday effect in magnetic insulators or semiconductors. However, there have been few reports on metals. Recently Choi et al. reported magnetization precession driven by the circularly-polarized light in ferromagnet/heavy metals bilayers [1]. They proposed new physics, optical spin-torque which is distinct from the traditional inverse Faraday effect. However, the physics of optical spin-torque is not clearly understood yet; thus, it is demanded to deeply understand the physics toward photo-spintronic applications. Here, we observed light-helicity induced magnetization precession in FeCo / Pt bilayers, which is found to be explained by the optical spin-torque. MgO / FeCo / Pt thin film were deposited on thermally oxidized Si substrate by a magnetron sputtering. The pulse width and wavelength of the femtosecond laser pulse used were 120 fs and 800 nm. Figure 1 shows the magnetization precession in FeCo / Pt bilayer with different light helicities, where 2 T in-plane magnetic field is applied. The solid curves in Fig. 1 show the fitting of sinusoidal function to the data. The phase of the magnetization precession has an information of a torque direction. Optical spin-torque is believed to be regarded as a damping-like torque, which is induced by a current of the spin-angular momentum in a nonmagnetic layer transferred from the circularly-polarized light and makes magnetization initailly tilt away from the film surface as shown in Fig. 2. It was found that the magnetization precession is mainly induced by the damping like-torque, however, we also observed field-like torque as a phase shift of the magnetization precession. The detailed discussion of field-like torque as well as its thickness dependence will be discussed in the presentation. This work was partially supported by KAKENHI (19K15430), Advanced Technology Institute Research Grants, and CSRN.References: [1] G. -M. Choi et al. Nat. Commun. 8, 15085 (2017), G. -M. Choi et al. Nat. Commun. 11, 1482 (2020). [2] S. Iihama and S. Mizukami, in-preparation.

Optical spin-torque in FeCo / Pt bilayer thin films

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SHORT BIO

Presentations

Laser induced terahertz wave emission from Bi/Co structure

Ultrafast Single Pulse All Optical Magnetization Switching of Ferromagnets

Interface optical spin generation in a ferromagnet/heavy metal heterostructure

Parity-controlled spin-wave excitations in synthetic antiferromagnets

Modulation of magnon-magnon coupling by inherent symmetry breaking in synthetic antiferromagnets

Optical spin-torque in FeCo / Pt bilayer thin films

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