GRAPHENE Graphene-Based Revolutions in ICT and Beyond Combination of CP and CSA. WP6 Graphene Spintronics

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1 GRAPHENE Graphene-Based Revolutions in ICT and Beyond Combination of CP and CSA WP6 Graphene Spintronics Deliverable 6.2 Proofs of concept of room temperature graphene spintronic device: A) Detection of magnetic field Main Author(s): Bart van Wees (RUG) Stephan Roche (ICN) Due date of deliverable: M12 Actual submission date: M12 Dissemination level: PU Project funded by the European Commission under grant agreement n

2 GRAPHENE D September / 9 LIST OF CONTRIBUTORS Partner Acronym Partner Name Name of the contact RUG Rijksuniversteit Groningen Bart van Wees CNRS Centre National de la Recherche Scientifique Pierre Seneor Albert Fert RWTH Rheinsch-Westfälische Technische Christoph Stampfer Hochschule Aachen Bernd Beschoten UBAS Universitaet Basel Christian Schoenenberger

3 GRAPHENE D September / 9 TABLE OF CONTENTS Deliverable Summary... 4 Introduction... 5 Optimization on the ferromagnetic contacts and contact fabrication procedure... 5 Development of new device geometries and transfer methods for improved spin transport... 7 Implications for the Hanle signal and magnetic field sensitivity... 7 Exploration of graphene based spintronic devices based on CVD and SiC graphene systems and graphene quantum dots... 8 Conclusions... 8 Publications related to this deliverable... 9

4 GRAPHENE D September / 9 Deliverable Summary This deliverable describes the first practical steps towards prototype graphene spintronic devices. As a first benchmark we will describe the progress in terms of the detection of magnetic fields. The detection of a (perpendicular) magnetic field is done via the induced Hanle spin precession of injected spin polarized carriers. This is analysed in the four-terminal non-local geometry, which allows to identify and quantify the spin related signals, and allows to exclude spurious effects. The magnetic field sensitivity depends on two important factors: The first is related to the specific spin transport parameters of the graphene: the spin relaxation length and the (spin) diffusion constant (the latter is related to the graphene mobility). Both determine the shape of the Hanle signal as a function of the magnetic field. In particular the width ΔB of the Hanle signal is inversely proportional to the spin relaxation time, and thus also determines the magnetic field sensitivity. The second factor is the (absolute) value of the spin signal. A crucial factor here is the spin injection efficiency of the contacts (and its sample-to-sample-variation/reproducibility) since the signal scales with the product of spin injection efficiency and detection efficiency. This deliverable describes the experimental progress in both areas, and how they result in the current magnetic field detection capabilities. Note that these developments are also crucial for the progress in the basic understanding of the fundamental spin relaxation mechanisms, which are highlighted and discussed in the parallel deliverable 6.1.

5 GRAPHENE D September / 9 Introduction Here we will describe two major technological steps to go towards optimized prototype graphene spintronic devices. This will be done by highlighting the observation of Hanle spin precession as a means to detect perpendicular magnetic fields. In this deliverable we will focus on: 1) The optimization of the ferromagnetic injector and detector (tunnel) contacts, both regarding spin injection/detection efficiency as well as reproducibility and potential for integration in large scale devices. 2) The optimization of the graphene spin carrying channel, in terms of spin relaxation time and mobility. Note here that these have implications for the typical device dimensions, since these are dictated by the spin relaxation length, which is determined itself by both the mobility as well as the spin relaxation time. Within the reporting period, our main goal was to develop technology to combine long spin relaxation time with large carrier mobilities at room temperature in non-local spin-valve devices. In this deliverable we will emphasize the practical aspects of device fabrication, and how they determine the magnetic field sensing properties. The determination and optimization of the spin transport parameters for the fundamental understanding of spin relaxation mechanisms will be discussed in the parallel deliverable 6.1 Optimization on the ferromagnetic contacts and contact fabrication procedure The RUG partner has continued to use Al 2 /O 3 barriers. They allow for typical spin polarizations of about 10%. This is enough for fundamental studies done in non-local 4 terminal devices, but will eventually not be enough to have a sufficient magnetoresistance ratio in two-terminal devices. Also the properties of these contacts vary, and they were found to deteriorate in atmospheric conditions. In this period the RUG partner focused however on the optimization of the spin transport in graphene in encapsulated graphene [1], which is described in deliverable 6.1. For their graphene-based spin transport devices the RWTH node has used Co/MgO electrodes for spin injection/detection. All their previous MgO x barriers were oxygen deficient. They have thus focused on improving the MgO stoichiometry as well as its structural quality (T6.1). They found that a postfabrication treatment of their devices in pure oxygen resulted in a strong improvement of spin transport properties which may result in an increase of both the spin relaxation time τ s and the spin resistance ΔR by factor of 7 reaching spin relaxation times above 1 ns. At the same time they observe an increase of the respective Co/MgO contact resistance area products R c A indicating that the spin transport parameters are currently limited by contact-induced spin dephasing and spin relaxation processes [2]. The UBAS node has worked on the optimization of tunnel barriers for spin injection, as part of T6.1[3]. For the tunnel barriers CVD hexagonal boron-nitride (h-bn) was used. Layered semiconductors offer homogenous tunnel barriers, as compared to oxide barriers made from thin oxidized metal layers, where inhomogeneous wetting of the grown layers on graphene can lead to pin-holes in the barrier. They found that the barrier resistance can be tuned by changing the number of h-bn layers. Already two layers offer a thick enough barrier to avoid conductance mismatch between the ferromagnetic

6 GRAPHENE D September /9 electrodes and graphene. UBAS has tested these barriers on both exfoliated and CVD grown graphene. They have found that even for CVD graphene devices with CVD h-bn barriers spinrelaxation times on the order of 300 pico-seconds can be achieved, a value that is similar to exfoliated samples on substrates (T3.1). The relaxation time was deduced from non-local TMR and Hanle measurements, which were performed both at 4K and at room temperature. They also measured local TMR, in which the resistance change appears at the same field as in the non-local measurement. The relation of two and four terminal signals is currently investigated. This kind of comparison might enable the understanding and the elimination of spurious effects in two-terminal samples. The fully CVD based approach offers the possibility for large scale fabrication for practical spintronics devices (D6.2, T6.5). They published our results on the full CVD approach recently [4]. Fig 1a) AFM and SEM images of SL h-bn transferred onto a SiO2/Si substrate. The arrows highlight triangular-shaped multi layered h-bn (red) and h-bn grain boundaries (white). Scale bar: 1 µm. b) Dependence of the resistance-area product RA on the number of transferred CVD h-bn layers. c) False coloured SEM image of a full-cvd device. Graphene is shown in blue, the ferromagnets in pink, whereas dark grey and gold are Pd and Ti/Au contacts, respectively. The whole graphene is covered by CVD h-bn. The width W of the graphene flake is 8 µm and the distance L between the two ferromagnetic contacts is 1 µm. The widths of the ferromagnetic Co electrodes are 150nm and 300 nm. d): Non-local and local signal shown in a full-cvd device with bilayer h-bn tunnel barriers. e) Hanle effect measured on device with channel of length 3 µm and bilayer h-bn barrier. (courtesy of UBAS)

7 GRAPHENE D September / 9 Development of new device geometries and transfer methods for improved spin transport The RWTH node has developed a new fabrication method of graphene spin-valve devices which yields enhanced spin and charge transport properties by improving both the electrode-to-graphene and graphene-to-substrate interface [4]. For this, they first prepare Co/MgO spin injection electrodes onto Si ++ /SiO 2. Thereafter, they mechanically transfer a graphene-hbn heterostructure onto the prepatterned electrodes. They showed that room temperature spin transport in single-, bi- and trilayer graphene devices exhibit nanosecond spin relaxation times with spin diffusion lengths reaching 10 µm combined with carrier mobilities exceeding 20,000 cm 2 /Vs (T6.1, 6.5). The corresponding long spin relaxation times is reflected in the relatively narrow Hanle signal (see fig. 2) Fig. 2 Left: Transfer technique for fabricating non-local graphene spin-valve devices. Right: Hanle spin precession curve for parallel and anti-parallel injector/detector magnetization configurations. (courtesy of RWTH) As a future experimental perspective (D6.1) we think that layered tunnel barriers combined with high mobility materials, realized for example by encapsulation of graphene, can give even longer spin relaxation times. One of the reasons for the decreased spin relaxation times in earlier measurements roots in part in the quality of the tunnel barriers and the tunnel barrier-ferromagnet interface. Using layered insulators like BN is a way to solve the former problem. The latter, however, has not been addressed by now. The ferromagnet-tunnel barrier interface can possibly be optimized by following the reversed fabrication method introduced by the RWTH team, in which the ferromagnets are fabricated first followed by the deposition of tunnel barriers. Similarly it is planned to combine the use of BN as barrier layer in the ferromagnetic contacts with the recently demonstrated enhancement of the spin relaxation time in BN encapsulated graphene (RUG), and the control of the spin relaxation by the (independent from charge density) electric field control of the spin relaxation in a dual-gate geometry. Implications for the Hanle signal and magnetic field sensitivity Fig. 2b illustrates a typical Hanle signal in a non-local spin valve device with a spin relaxation time in the range of 2 ns. The width ΔB is about 20 mt and is one of the narrowest observed so far. It shows that the spin signal can be changed by an applied perpendicular magnetic field from a full signal at 0T

8 GRAPHENE D September / 9 to zero at about 20 mt. The magnitude of the signal is relatively small (0.4 Ω) because the contact polarization was not optimized in these experiments. We believe it will be possible to obtain signals in the order of 100 Ω or more, with a similar magnetic field sensitivity. Exploration of graphene based spintronic devices based on CVD and SiC graphene systems and graphene quantum dots The CNRS node is experimentally studying the spin transport properties of large scale graphene readily compatible with further device integration. In the continuation of our previous results which have shown that epitaxial graphene on SiC (C face) is able to provide large spin signals [5], a collaboration with Flagship partner Institut Néel/Georgia Tech (C. Berger/W. de Heer) is pursued to deepen our understanding of epitaxial graphene spin transport properties with the development of novel spin injectors. In parallel, our efforts focus on wafer-scale graphene monolayers grown by Chemical Vapor Deposition (CVD) for which a high quality catalytic growth on Cu has been previously developed in collaboration with the University of Cambridge (dept. of Eng.) [6]. Our goal is not only to further understand spin transport in graphene and to clearly highlight the different regimes of spin injection/transport [7], but more specifically to reach high efficiency spin transport within monolayer graphene channels, paving the ground for the next step: spin manipulation studies. In parallel, CNRS studies a novel approach to integrate graphene layers into spintronics devices. They developed the growth of graphene directly on top of spin sources by a CVD process [8], unlocking new wet/ambient processes for spintronics (such as Atomic Layer Deposition) and uncovering a novel strong spin-filtering effect at the graphene/ferromagnet interface [9]. Current developments concern the study of high quality graphene monolayers grown epitaxially on monocrystaline Ni(111) films [10]. Finally we note that it is expected that due to (quantum) confinement the spin relaxation times will be longer in graphene quantum dots than in extended 2D graphene devices. This would be favourable for magnetic field detection. RWTH has made progress in the fabrication of BN supported graphene quantum dots, but no results on spin relaxation are available yet. Conclusions In the past year rapid progress was made in the optimization of the graphene spin transport properties and the technology for optimized contacts. We believe however that considerable further improvements can be made, and we will now also focus on a integration of the various technologies for an optimized prototype.

9 GRAPHENE D September / 9 Publications related to this deliverable 1) M. Guimaraes et al, Phys. Rev. Lett 113, (2014) 2) F. Volmer, et al., arxiv: , accepted for publication in Phys Rev. B (2014). 3) W. Fu et al., J. Appl. Phys 116, (2014) 4) M. Drögeler, et al. arxiv: , accepted for publication in Nano Letters (2014). 5) Dlubak et al. Nature Physics 8, 557 (2012) 6) Kidambi et al., J Phys Chem C 116, (2012) 7) Seneor et al., MRS Bull. 37, 1245 (2012) 8) Dlubak et al., ACS Nano 6, (2012) 9) Martin et al., ACS Nano 8, 7890 (2014) 10) Weatherup et al. JACS (2014)

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