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Non-destructive imaging for buried interfaces has been recently developed by decelerating electron-beam energy in scanning electron microscope (SEM) [1]. This imaging technique has proven to be very useful to identify the contaminations formed in a magnetic tunnel junctions (MTJs), which reduce their tunnelling magnetoresistance (TMR) ratios. For example, in a Heusler-alloy MTJ, residual resist has been found to react with Al during Al-O sputtering for the isolatation of the top and bottom electrodes. By reducing the Al-O sputtering power, the yield of the MTJs has been reported to be improved over 70% [2]. In order to further evaluate the resolution of this technique, we prepared a new set of samples with elevating capping layers in this study. The samples, consisting of Ta (5)/(Ru (5)/)W or Pt (0.5)/Ta (5~60) (thickness in nm), were deposited on Si substrates using a high target utilisation sputtering system. Here, the heavy metal layer of W or Pt were intrinsically dispersed as nano-particles. Their diameters were evaluated by imaging with the non-destructive technique, confirming the resolution. The penetration depth of the electron beam in SEM with different energy was estimated using CASINO programme [3]. The electron beam at 4.7 keV is found to reach the interface between Pt and Ta for the case of the 60 nm thick Ta capping layer and to generate back scattered electrons (BSE). The electron beam at 5.0 keV, on the other hand, is found to reach the bottom Pt (or W) interface and to generate BSE. By subtracting these images, the distribution of the Pt nano-particles can be assessed. The corresponding SEM image taken by the subtraction of these acceleration voltages can resolve the Pt nano-particles with 10 nm diameter. For the case of the 5 nm thick Ta capping layer, 2 nm resolution is achieved. Such resolution can be useful for the evaluation of buried MTJs with a few 10 nm diameter. We will further improve the resolution by optimising the imaging conditions, so that we will be able to image smaller MTJs. This work is partially supported by EPSRC-JSPS Core-to-Core programme (EP/M02458X/1) and JST CREST (JPMJCR17J5).References: [1] A. Hirohata et al., Nat. Commun. 7, 12701 (2016). [2] E. Jackson et al., Sci. Rep. 8, 7585 (2018). [3] D. Drouin et al., Scanning 29, 92 (2007).

MMM 2020

Resolution of Non-Destructive Imaging for Buried Interfaces

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The recent discovery that van der Waals-bonded magnetic materials retain long range magnetic ordering down to a single layer[1,2] stimulates a thorough Raman spectroscopic study of one such material, FePS3, a large spin (S = 2) Mott insulator where the Fe atoms form a honeycomb lattice. Bulk FePS3 was shown to be a quasi-2D Ising antiferromagnet, with additional features in the Raman spectra emerging below the Neel temperature (TN ~ 120 K). Using temperature- and magnetic field-dependent Raman spectroscopy as an optical probe of magnetic structure, we demonstrate[3] that one of these Raman-active modes (ψ4) below TN is a magnon with a frequency of ~ 3.7 THz (~122 cm-1). Contrary to previous work[4], which interpreted this feature as a phonon, our Raman data[3] shows the expected frequency shifting and splitting of the magnon as a function of temperature and magnetic field, respectively, were we find the g-factor ~2. Other Raman-active modes emerging below TN are attributed to zone-folded phonons in the antiferromagnetic state. The anomalous temperature dependence of these modes along with an analysis of temperature-dependent magnetization data, suggests a persistence of short-range magnetic order above TN.References: [1] C. Gong, L. Li, Z. Li, et al., Nature 546, 265 (2017). [2] B. Huang, G. Clark, E. Navarro-Moratalla, et al., Nature 546, 270 (2017). [3] A. McCreary, J. R. Simpson, T. T. Mai, et al., Phys. Rev. B 101, 064416 (2020). [4] J.-U. Lee, S. Lee, S. H. Ryoo, et al., Nano Lett. 16, 7433 (2016).

Temperature- and Magnetic Field-Dependent Raman Spectroscopy of Layered, Antiferromagnetic FePS3

Material structures containing tetrahedral FeAs bonds, depending on their density and geometrical distribution, can host several competing quantum ground states ranging from superconductivity to ferromagnetism. In Fe-based superconductors where the FeAs bonds are confined in 2D monolayers (MLs), the magnetic ground state of the Fe spins is antiferromagnetic1. On the other hand, in Fe-based ferromagnetic semiconductors such as (In,Fe)As where the FeAs bonds are distributed randomly in a three-dimensional (3D) InAs matrix, the Fe spins are coupled ferromagnetically via interactions with electron carriers2. Here we examine structures of quasi two-dimensional (2D) layers of tetrahedral FeAs bonds embedded with a regular interval in a semiconductor InAs matrix, which resemble the crystal structure of Fe-based superconductors. The samples were grown by low-temperature molecular beam epitaxy on InAs (001) or semi-insulating GaAs (001) substrates. Lattice images by scanning transmission electron microscopy (STEM) reveal that the zinc-blende structure of the host InAs is well maintained, and the Fe atoms are mainly confined within a thickness of 2-3 MLs (Fig. 1a). We study magnetic and transport properties of a series of FeAs/InAs superlattices (thickness is fixed at 12 nm) containing (1ML of FeAs / t ML of InAs) x N periods (t = 20, 10, 7, 5; N = 1, 3, 5, 7) (the inset of Fig. 1(b)). All the samples exhibit intrinsic ferromagnetism, and the TC value changes rapidly as t-3 (Fig 1b). Furthermore, extremely large magnetoresistance (MR) (~500%, Fig. 1c) are observed, whose origin can be attributed to the giant MR occurring in these multilayer structures. These interesting features indicate that the FeAs/InAs superlattice structures are promising for functional spintronic devices3. This work was partly supported by Grants-in-Aid for Scientific Research (17H04922, 18H05345, 19H05602, 19K21961), CREST program (JPMJCR1777) and PRESTO program (JPMJPR19LB) of JST, and Spin-RNJ.References: [1] H. Hosono et al. Materials Today 21, 278-302 (2018). [2] P. N. Hai, L. D. Anh et al., Appl. Phys. Lett. 101, 182403 (2012). [3] L. D. Anh et al, ArXiv:2005.10181 (2020).

Ferromagnetism and giant magnetoresistance in zinc-blende FeAs/InAs superlattice structures

The proximity effect in two-dimensional materials opens ways to achieve important functions for future spintronic devices. In van der Waals heterostructures (vdWHs), transition metal dichalcogenides (TMD) can be used to enhance the spin-orbit coupling of graphene leading to highly efficient spin-to-charge conversion (SCC) by spin Hall effect (SHE) that is predicted to be controllable by a gate voltage. Here, we report for the first time the observation of the SHE in graphene proximitized with WSe2 in a vdWHs. These kind of vdWHs are a promising platform to study a variety of spin-dependent phenomena [1,2]. By Hanle precession measurements, we quantify the spin transport and SCC parameters from 10 K up to room temperature. Exceptional for graphene/TMD devices, the sole mechanism is the SHE for all measurements and no Rashba-Edelstein effect is observable. Importantly, we are able to amplify and turn off the SCC by applying a back-gate voltage, demonstrating the long-awaited milestone of an electrically-tunable SHE. The amplified SCC shows a high efficiency, measured with an unprecedented SCC length of larger than 20 nm, defined as the product of the spin Hall angle (ΘSH) and the spin diffusion length (λs). These results show the capability of two-dimensional materials to advance towards the implementation of novel spin-based devices and future applications.References: [1] W. Yan et al., Nat. Commun. 7, 13372 (2016). [2] C. K. Safeer et al., Nano Lett. 19, 1074–1082 (2019).

Proximity-Induced Spin Hall Effect in Graphene/WSe2 van der Waals Heterostructures with Tunable, Highly Efficient Spin-to-Charge Conversion

Recently, van-der-Waals (vdW) magnets have attracted much attention and been researched extensively [1]. The present study aims to elucidate the magnetic properties of a vdW magnet, namely CeTe3. CeTe3 is a cleavable magnetic material in the family of rare earth tritellurides. Its crystal structure consists of a CeTe slab, separated by two Te layers. The material undergoes two magnetic phase transitions at TN1 = 3 K and TN2 = 1.2 K. For bulk CeTe3, the first transition is understood to be to an antiferromagnetic (AFM) state with an in-plane easy axis [2, 3]. The second transition is known to be to a different AFM state with still an in-plane easy axis, but a nonparallel axis to the first AFM state [4]. However, details of these AFM states are still unknown, and thin film transport measurements have not been performed yet. In this work, we have performed magnetoresistance measurements from 0.4 to 4 K on 40 nm CeTe3 thin film devices [5]. Figure 1 shows magnetoresistance at different temperatures. We have observed a clear Shubnikov-de-Haas oscillation from well above TN1, which has never been reported so far. Such a large oscillation implies a highly two-dimensional (2D) nature of the electrical conduction. Moreover, we have observed a unique hysteresis and peak structure below TN1 which is retained even below TN2, as shown in Fig. 2. This implies a possible canting of the magnetic moments along the stacking direction induced through the thin film fabrication. Further studies could lead to understanding the possible enhancement of perpendicular magnetic anisotropy in magnetic thin films. Moreover, the coexistence of quantum oscillation and magnetic hysteresis is extremely unique, and the material would pave the way for understanding the interaction between magnetic moments and highly 2D conduction electrons.References: [1] Y. Deng et al., Nature 563, 94 (2018) [2] Y. Iyeiri et al., Phys. Rev. B 67, 144417 (2003). [3] K. Deguchi et al., J. Phys.: Conf. Ser. 150, 042023 (2009). [4] D. A. Zocco et al., Phys. Rev. B 79, 134428 (2009). [5] M. Watanabe et al., arXiv: 2006.14955.

Coexistance of quantum oscillation and magnetic hysteresis in CeTe3 thin films

The use of double magnetic tunnel junctions (DMTJ) is a well-known strategy to enhance STT-MRAM efficiency by increasing thermal stability (Δ) while reducing the critical switching current (Ic). In these structures, the Storage layer (SL) is sandwiched between two tunnel barriers, each with its corresponding fixed polarizer. For the case of perpendicular DMTJ, the SL Δ is increased due to the two interfacial anisotropy contributions arising from both magnetic metal-oxide interfaces. If the top (TP) and bottom (BP) polarizers are set antiparallel, the Ic is found both theoretically [1] and experimentally [2] to be reduced due to additive spin-transfer torques. Another feature of DMTJ is the possibility of switching one of the polarizers, allowing to tune the STT depending on the polarizers parallel (Read Mode) or antiparallel (Write Mode) configuration [3]. Fig.1 (a) and (b) show the structure of such p-DMTJ with switchable TP and the two operation modes, where the polarizers are coupled to a hard Co/Pt synthetic antiferromagnetic multilayer (SAF). In this study, we investigate the possibility of replacing the TP SAF by a single magnetic layer realizing a p-DMTJ structure as depicted in Fig.1.(c). The structure proposed comprises a SAF based BP acting also as a fixed reference layer, a composite SL and the top free polarizer called assistance layer (ASL). The ASL is designed to have an out-of-plane anisotropy and a coercivity lower than that of the SL. In standby, the magnetic coupling between the SL and the ASL sets the magnetization of these two layers in parallel configuration, reinforcing the Δ of the SL. During write, the ASL acts as a polarizer inducing an additional STT, thus reducing the Ic. To investigate this concept, we fabricated, characterized and modeled these devices to understand the ASL working conditions. We demonstrate an increase by a factor of 5 in the figure of merit Δ/Ic of these structures compared to conventional MTJ stack for STT-MRAM with double barriers and a non-magnetic ASL Fig.2.References: [1] Daniel C. Worledge,IEEE MAGNETICS LETTERS, Volume 8 (2017) [2] G. Hu, J. H. Lee, J. J. Nowak, IEEE International Electron Devices Meeting (IEDM), (2015) [3] P.-Y. Clément, C. Baraduc, M. Chshiev, B. Diény,IEEE 6th International Memory Workshop (IMW), (2014) [4] K. Nishioka, H. Honjo, S. Ikeda,Symposium on VLSI Technology Digest of Technical Papers, (2019)

Simplified Double Magnetic Tunnel Junction with switchable Assistance layer for improved STT-MRAM performance

CoFeB-MgO-based magnetic tunnel junctions (MTJs) with perpendicular magnetic anisotropy (PMA) (p-MTJs) [1-3] have become the de-facto standard of current STT-MRAM. In the STT-MRAM, the bottom pinned structure [4,5], and in the SOT-MRAM, the top pinned structure has been employed [6,7]. The bottom pinned structure exhibits high PMA, whereas the top pinned structure is difficult to obtain a high PMA of Co/Pt due to the unavailability of a thick buffer layer under Co/Pt. In the bottom pinned p-MTJs, as the Pt buffer layer thickness increases, the PMA of Co/Pt increases [8]. However, Pt thickness cannot exceed 2 nm to obtain sufficient magnetic coupling between ferromagnetic layers [9]. Therefore, there is a trade-off between PMA and magnetic coupling in the top pinned structure. To overcome this trade-off, we developed a high PMA Co/Pt pinned layer for top pinned p-MTJs, using surface modification treatment (SMT). In Stack A without SMT, Pt seed layer (SL) thickness varied from 0.5 to 2.5 nm. In Stack A with SMT, a 6 nm-thick Pt SL was exposed to Ar ion plasma. After SMT, the residual Pt SL thickness was varied from 0.5 to 2.5 nm. We also prepared top pinned p-MTJs (Stack B) with a synthetic ferrimagnetic structure with and without SMT (Fig.2(a)). Annealing temperature is 300, 350, and 400°C for 1 h. In Stack A with SMT, the values of magnetic anisotropy energy density Keff*t are larger than those without SMT (Fig.1). In Stack B with SMT, TMR ratio increases up to 400°C, whereas in Stack B without SMT, TMR ratio degrades at 400°C (Fig.2(b)). The employment of SMT is very effective for achieving both higher perpendicular anisotropy and robustness against annealing for top pinned structure. This work is supported by CIES’s Industrial Affiliation on STT MRAM program, CIES Consortium, JST-OPERA, and CAO-SIP.References: [1] S. Ikeda et al., Nature Mater. 9, 721 (2010). [2] H. Sato et al., Appl. Phys. Lett. 101, 022414 (2012). [3] H. Sato et al., IEEE Trans. Magn. 49, 4437 (2013). [4] H. Honjo et al., J. Appl. Phys., 126, 113902 (2019). [5] K. Nishioka et al., IEEE Trans Electron Devices 67, 995 (2020). [6] H. Honjo et al., IEDM, 28.5.1. (2019). [7] M. Natsui et al., VLSI, CM2.2 (2020). [8] H. Honjo et., al, VLSI, T160 (2015). [9] H. Honjo et., al, IEEE Trans. Magn. 50, 1401904 (2014).

Effect of surface modification treatment on top pinned MTJ with perpendicular easy axis

A major obstacle to reliable and fast STT-induced switching is a counterintuitive phenomenon: the back-hopping (BH). We generally expect that the switching probability should always increase with the applied voltage. However the contrary can sometimes occur: in many instances, the MTJ resistance can back-hop to its original state after the apparent successful switching of the FL magnetization, as in the STT loop in Figure 1 at large positive voltage bias. We analyze the BH phenomenon in STT induced switching of perpendicularly magnetized tunnel junctions mimicking state-of-the art STTMRAM cells. The analysis is based on single-shot nanosecond time-resolved conductance measurements of the pulse-induced BH. The protocol allows to assign the conductance dynamics to the sole magnetization dynamics by avoiding the contributions from the bias dependence of the conductance and from current-induced heating. Studying several material variants reveals that the back-hopping is a feature of the nominally fixed system of the tunnel junction. This rules out earlier proposed scenarios based on the switching back of the free layer as a result of some anomalous voltage dependence of the STT acting on the free layer. The back-hopping is found (figure) to proceed by two sequential switching events that lead to a final state P' of conductance close to --but distinct from-- that of the conventional parallel state. The P' state does not exist at remanence. It generally relaxes to the conventional antiparallel state if the current is removed. The P' state involves a switching of the sole spin-polarizing part of the fixed layers, i.e. the barrier-facing part of the fixed layers. The analysis of our several material variants indicates that back-hopping occurs only when the spin-polarizing layer is too weakly coupled to the rest of the fixed system. This provides mitigation strategies of back-hopping for next generation STTMRAMs.References: T. Devolder et al, arXiv:2006.05108.

Back-hopping in Spin-Transfer-Torque switching of perpendicularly magnetized tunnel junctions

Magnetic tunnel junctions (MTJs) with perpendicular magnetic anisotropy (PMA) have been studied in the recent decades as the crucial element for next generation memory applications [1]. As the data-storage layer in MTJs, the dual-MgO free layers (FLs) with a structure as MgO/CoFeB/spacer/CoFeB/MgO have been under intense development to provide high PMA and low damping after annealing, which guarantees the high thermal stability and low switching current in MTJ devices [2]. The previous efforts for the optimization of dual-MgO FLs include the engineering of non-magnetic spacer [3-5] and boron composition [6]. As a novel approach, we explore the impact of Fe80B20 inserted at both Co20Fe60B20/MgO interfaces of dual-MgO FLs under different annealing conditions in bottom-pinned MTJs. Current-in-plane tunnelling measurements are carried out to characterize magnetotransport properties of the MTJs. Conventional magnetometry measurements and ferromagnetic resonance are conducted to estimate the PMA and the Gilbert damping of dual-MgO FLs as a function of the Fe80B20 thickness and annealing temperatures. With ultrathin Fe80B20 (0.2 - 0.4 nm) inserted at the bottom interface, the tunnel magneto-resistance (TMR) can be maintained with a lower resistance-area (RA) product, while the top-FeB insertion results in a more RA drop with a similar TMR (Fig. 1(a)). The PMA of dual-MgO FLs with FeB inserted at the bottom interface shows a larger improvement than its top FeB insertion counterpart, even after 400 °C annealing (Fig. 1(b,c)). At the same time, the ultrathin FeB insertion at either interface reduces the damping constant in the FL (Fig. 1(d,e)). By optimizing the FeB insertion layer thickness and location, dual-MgO FLs with an unchanged TMR, higher effective anisotropy and lower damping can be achieved. This study demonstrates a novel approach to tune properties of dual-MgO FLs up to 400 °C annealing, which enables MTJ stacks for various applications.References: [1] Ikeda S, et al. 2010 Nat. Mater. 9 721–4 [2] Sato H, et al. 2014 Appl. Phys. Lett. 105 062403 [3] Liu T, et al. 2015 Sci. Rep. 4 5895 [4] Couet S, et al. 2016 IEEE Magn. Lett. 7 3103004 [5] Chatterjee J, et al. 2017 Appl. Phys. Lett. 110 202401 [6] Honjo H, et al. 2016 IEEE Trans. Magn. 52 1–4

Impact of Fe80B20 insertion on the properties of dual-MgO perpendicular magnetic tunnel junctions

Development of CoFeB/MgO based magnetic tunneling junction with perpendicular magnetic anisotropy (PMA) (p-MTJ) [1] has greatly contributed to realize the mass production of STT-MRAM. The higher thermal stability factor (△) is required for further scaling down of MTJ. In order to achieve high △, double and quad CoFeB/MgO interfaces p- MTJs have been proposed [2-4]. Single thin nonmagnetic layer (e.g., Ta, W, MgO, etc.) is inserted in the free layer to obtain high PMA (Stack A in Fig.1) [2]. In addition, enhancement of magnetic coupling (Jcpl) between free layer 1 and free layer 2 is also important to increase △, because △ does not increase when the magnets behave magnetically independently without Jcpl. Previous study showed an enhancement of PMA in double interface p-MTJ by inserting a thin ferromagnetic layer sandwiched by two nonmagnetic layers in the free layer [5] (we call as “ferromagnetic bridge layer (FBL)”). However, Jcpl for the free layer with FBL was not considered. In this study, we investigated Kefft* and Jcpl for the free layer with FBL in the double interface p-MTJ and simulated its impact on △. We prepared two types of stack with single insertion layer (Stack A) and FBL (Stack B). All stacks were deposited by DC/RF magnetron sputtering system, and then annealed at 400oC for 1h. Figures1-2 show experimental results of total insertion layer thickness (t) dependence of Jcpl and Kefft*. Stack B with FBL showed higher Kefft* than Stack A with single insertion layer in all t range, while keeping higher Jcpl when t was up to 0.5 nm because each insertion layer thickness is much thinner than single insertion layer. This could result in higher △ in Stack B with FBL because △ is proportional to Kefft* and effective free layer volume. Detailed simulation method and results will be presented. The FBL structure is an important technology to achieve high values both in Jcpl and Kefft*, which result in high △ for double and quad CoFeB/MgO interfaces MTJ. This work is supported by CIES’s Industrial Affiliation on STT MRAM program, CIES Consortium, JST-OPERA, and CAO-SIP.References: [1] S. Ikeda et al., Nat. Mater. 9, 721 (2010). [2] H. Sato et al., Appl. Phys. Lett. 101, 022414 (2012). [3] H. Honjo et al., Dig. Tech. Pap. Symp. VLSI Technology, 2015, T160. [4] K. Nishioka et at., IEEE Trans. Electron Devices 67, 995 (2020). [5] J. Chatterjee at al., Phys Rev. Appl 12, 044043 (2019). [6] G. D. Chaves-O’Flynn et al., Phys. Rev. Appl. 4, 024010 (2015).

Enhancement of magnetic interaction and magnetic anisotropy in MTJ with multiple CoFeB/MgO interfaces for high thermal stability

Magnetic random access memory (MRAM) devices are envisioned as a major candidate for future memory technologies. Using an exchange coupled composite free layer (ECC FL) for perpendicular magnetic tunnel junction can improve the operation as predicted by a two-spin model [1]. Here, we show that ECC FL leads to significant reduction of the switching current and increase of the efficiency defined as the ratio between the energy barrier and switching current for device sizes (20-50nm) when the magnetization dynamics can be non-uniform. The results are obtained via the micromagnetic simulations performed with the micromagnetic simulator FastMag [2]. Figure 1 shows the thermal stability factor Δ and switching current density Jc0 as a function of the surface exchange energy density Jex for different anisotropy ratios γ between the ECC sublayers (i.e. FLsoft and FLhard ). of the ECC FL. The thermal stability factor increases with Jex (Fig. 1a). The switching current density Jc0 has an optimal value of the Jex at which it is minimal (Fig. 1b). The reduction of Jc0 is greater for greater γ and it can be reduced more than half as compared to a regular FL. The corresponding efficiency exhibits the maximal improvement of over 1.65 as compared to a regular FL. The mechanism leading to these improvements is that the switching of the softer layer assists in the switching of the harder layer. It is important that the reference layer is next to the softer layer. We find that the devices of a smaller size need to have a significantly greater surface coupling strength to achieve optimal operation. Support from the Semiconductor Research Corporation is greatly acknowledged.References: [1] I. Yulaev, M. V. Lubarda, S. Mangin, V. Lomakin, E. E. Fullerton, APL 99 (13), 132502 (2011). [2] R. Chang, S. Li, M. V. Lubarda, B. Livshitz, and V. Lomakin, J Appl Phys 109 (3), 07D358 (2011).

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