Substrate-assisted nucleation of ultra-thin dielectric layers on graphene by atomic layer deposition

We report on a large improvement in the wetting of Al2O3 thin films grown by un-seeded atomic layer deposition on monolayer graphene, without creating point defects. This enhanced wetting is achieved by greatly increasing the nucleation density through the use of polar traps induced on the graphene surface by an underlying metallic substrate. The resulting Al2O3/graphene stack is then transferred to SiO2 by standard methods.P.R.K. acknowledges funding from Cambridge Commonwealth Trust. R.S.W. acknowledges funding from EPSRC (Doctoral training award). S.H. acknowledges funding from ERC Grant InsituNANO (No. 279342) and EPSRC (Grant No. EP/ H047565/1).This is the accepted manuscript. The final version is available from AIP from http://scitation.aip.org/content/aip/journal/apl/100/17/10.1063/1.4707376

The parameter space of graphene chemical vapor deposition on polycrystalline Cu

A systematic study on the parameter space of graphene CVD on polycrystalline Cu foils is presented, aiming at a more fundamental process rationale in particular regarding the choice of carbon precursor and mitigation of Cu sublimation. CH4 as precursor requires H2 dilution and temperatures ≥1000°C to keep the Cu surface reduced and yield a high quality, complete monolayer graphene coverage. The H2 atmosphere etches as-grown graphene, hence maintaining a balanced CH4/H2 ratio is critical. Such balance is more easily achieved at low pressure conditions, at which however Cu sublimation reaches deleterious levels. In contrast, C6H6 as precursor requires no reactive diluent and consistently gives similar graphene quality at 100-150°C lower temperatures. The lower process temperature and more robust processing conditions allow the problem of Cu sublimation to be effectively addressed. Graphene formation is not inherently self-limited to a monolayer for any of the precursors. Rather, the higher the supplied carbon chemical potential the higher the likelihood of film inhomogeneity and primary and secondary multilayer graphene nucleation. For the latter, domain boundaries of the inherently polycrystalline CVD graphene offer pathways for a continued carbon supply to the catalyst. Graphene formation is significantly affected by the Cu crystallography, i.e. the evolution of microstructure and texture of the catalyst template form an integral part of the CVD process.S.H. acknowledges funding from ERC grant InsituNANO (n°279342) and from EPSRC (Grant Nr. EP/H047565/1). P.R.K. acknowledges funding from the Cambridge Commonwealth Trust and C.D. acknowledges funding from Royal Society.This is the accepted manuscript. The final version is available from ACS at http://pubs.acs.org/doi/abs/10.1021/jp303597m

Measuring the nonlinear refractive index of graphene using the optical Kerr effect method

© 2016 Optical Society of America.By means of the ultrafast optical Kerr effect method coupled to optical heterodyne detection (OHD-OKE), we characterize the third-order nonlinear response of graphene and compare it to experimental values obtained by the Z-scan method on the same samples. From these measurements, we estimate a negative nonlinear refractive index for monolayer graphene, n2 = -1.1 × 10-13 m2/W. This is in contradiction to previously reported values, which leads us to compare our experimental measurements obtained by the OHD-OKE and the Z-scan method with theoretical and experimental values found in the literature and to discuss the discrepancies, taking into account parameters such as doping

WS2 2D Semiconductor Down to Monolayers by Pulsed-Laser Deposition for Large-Scale Integration in Electronics and Spintronics Circuits

We report on the achievement of a large-scale tungsten disulfide (WS2) 2D semiconducting platform derived by pulsed-laser deposition (PLD) on both insulating substrates (SrTiO3), as required for in-plane semiconductor circuit definition, and ferromagnetic spin sources (Ni), as required for spintronics applications. We show thickness and phase control, with highly homogeneous wafer-scale monolayers observed under certain conditions, as demonstrated by X-ray photoelectron spectroscopy and Raman spectroscopy mappings. Interestingly, growth appears to be dependent on the substrate selection, with a dramatically increased growth rate on Ni substrates. We show that this 2D-semiconductor integration protocol preserves the interface integrity. Illustratively, the WS2/Ni electrode is shown to be resistant to oxidation (even after extended exposure to ambient conditions) and to present tunneling characteristics once integrated into a complete vertical device. Overall, these experiments show that the presented PLD approach used here for WS2 growth is versatile and has a strong potential to accelerate the integration and evaluation of large-scale 2D-semiconductor platforms in electronics and spintronics circuits

Graphene-passivated nickel as an oxidation-resistant electrode for spintronics.

We report on graphene-passivated ferromagnetic electrodes (GPFE) for spin devices. GPFE are shown to act as spin-polarized oxidation-resistant electrodes. The direct coating of nickel with few layer graphene through a readily scalable chemical vapor deposition (CVD) process allows the preservation of an unoxidized nickel surface upon air exposure. Fabrication and measurement of complete reference tunneling spin valve structures demonstrate that the GPFE is maintained as a spin polarizer and also that the presence of the graphene coating leads to a specific sign reversal of the magneto-resistance. Hence, this work highlights a novel oxidation-resistant spin source which further unlocks low cost wet chemistry processes for spintronics devices.R.S.W. acknowledges funding from EPSRC (Doctoral training award). S.H. acknowledges funding from ERC Grant InsituNANO (Project Reference 279342). P.S. acknowledges the Institut Universitaire de France for junior fellowship support. This research was partially supported by the EU FP7 work programme under Grant GRAFOL (Project Reference 285275).This is the accepted manuscript. The final version is available from ACS at http://pubs.acs.org/doi/abs/10.1021/nn304424x

A perpendicular graphene/ferromagnet electrode for spintronics

We report on the large-scale integration of graphene layers over a FePd perpendicular magnetic anisotropy (PMA) platform, targeting further downscaling of spin circuits. An L10 FePd ordered alloy showing both high magneto-crystalline anisotropy and a low magnetic damping constant, is deposited by magnetron sputtering. The graphene layer is then grown on top of it by large-scale chemical vapor deposition. A step-by-step study, including structural and magnetic analyses by x-ray diffraction and Kerr microscopy, shows that the measured FePd properties are preserved after the graphene deposition process. This scheme provides a graphene protected perpendicular spin electrode showing resistance to oxidation, atomic flatness, stable crystallinity, and perpendicular magnetic properties. This, in turn, opens the way to the generalization of hybrid 2D-materials on optimized PMA platforms, sustaining the development of spintronics circuits based on perpendicular spin-sources as required, for instance, for perpendicular-magnetic random-access memory schemes

Atomic layer deposition of a MgO barrier for a passivated black phosphorus spintronics platform

We demonstrate a stabilized black phosphorus (BP) 2D platform thanks to an ultrathin MgO barrier, as required for spintronic device integration. The in-situ MgO layer deposition is achieved by using a large-scale atomic layer deposition process with high nucleation density. Raman spectroscopy studies show that this layer protects the BP from degradation in ambient conditions, unlocking in particular the possibility to carry out usual lithographic fabrication steps. The resulting MgO/BP stack is then integrated in a device and probed electrically, confirming the tunnel properties of the ultrathin MgO contacts. We believe that this demonstration of a BP material platform passivated with a functional MgO tunnel barrier provides a promising perspective for BP spin transport devices

Protecting nickel with graphene spin-filtering membranes: A single layer is enough

We report on the demonstration of ferromagnetic spin injectors for spintronics which are protected against oxidation through passivation by a single layer of graphene. The graphene monolayer is directly grown by catalytic chemical vapor deposition on pre-patterned nickel electrodes. X-ray photoelectron spectroscopy reveals that even with its monoatomic thickness, monolayer graphene still efficiently protects spin sources against oxidation in ambient air. The resulting single layer passivated electrodes are integrated into spin valves and demonstrated to act as spin polarizers. Strikingly, the atom-thick graphene layer is shown to be sufficient to induce a characteristic spin filtering effect evidenced through the sign reversal of the measured magnetoresistance.We acknowledge the Helmholtz-Zentrum-Berlin Electron storage ring BESSY II for provision of synchrotron radiation at the ISISS beamline and we thank the BESSY staff for continuous support of our experiments. R.S.W. acknowledges a Research Fellowship from St. John’s College, Cambridge. S.H. acknowledges funding from ERC grant InsituNANO (No. 279342) and EPSRC grant GRAPHTED (EP/K016636/1). P.S. acknowledges the Institut Universitaire de France for a junior fellowship. This research was partially supported by the EU FP7 Work Programme under Grant GRAFOL (No. 285275) and Graphene Flagship (No. 604391).This is the final published version. It first appeared at http://scitation.aip.org/content/aip/journal/apl/107/1/10.1063/1.4923401

Spin filtering by proximity effects at hybridized interfaces in spin-valves with 2D graphene barriers.

We report on spin transport in state-of-the-art epitaxial monolayer graphene based 2D-magnetic tunnel junctions (2D-MTJs). In our measurements, supported by ab-initio calculations, the strength of interaction between ferromagnetic electrodes and graphene monolayers is shown to fundamentally control the resulting spin signal. In particular, by switching the graphene/ferromagnet interaction, spin transport reveals magneto-resistance signal MR > 80% in junctions with low resistance × area products. Descriptions based only on a simple K-point filtering picture (i.e. MR increase with the number of layers) are not sufficient to predict the behavior of our devices. We emphasize that hybridization effects need to be taken into account to fully grasp the spin properties (such as spin dependent density of states) when 2D materials are used as ultimately thin interfaces. While this is only a first demonstration, we thus introduce the fruitful potential of spin manipulation by proximity effect at the hybridized 2D material / ferromagnet interface for 2D-MTJs