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Controlling magnetic properties through the application of an electric field is a significant challenge in modern nanomagnetism. In this study, we investigate the magneto-ionic control of magnetic anisotropy in the topmost Co layer in Ta/Pt/[Co/Al/Pt]$_n$/Co/Al/AlO$_\text{x}$ multilayer stacks comprising $n +1$ Co layers and its impact on the magnetic properties of the multilayers. We demonstrate that the perpendicular magnetic anisotropy can be reversibly quenched through gate-driven oxidation of the intermediary Al layer between Co and AlO$_\text{x}$, enabling dynamic control of the magnetic layers contributing to the out-of-plane remanence - varying between $n$ and $n +1$. For multilayer configurations with $n = 2$ and $n = 4$, we observe reversible and non-volatile additions of 1/3 and 1/5, respectively, to the anomalous Hall effect amplitude based on the applied gate voltage. Magnetic imaging reveals that the gate-induced spin-reorientation transition occurs through the propagation of a single 90$^{\circ}$ magnetic domain wall separating the perpendicular and in-plane anisotropy states. In the 5-repetition multilayer, the modification leads to a doubling of the period of the magnetic domains at remanence. These results demonstrate that the magneto-ionic control of the anisotropy of a single magnetic layer can be used to control the magnetic properties of coupled multilayer systems, extending beyond the gating effects on a single magnetic layer., Comment: 9 pages + 3 pages of supplementary materials, 5 main figures + 6 supplementary figures

Black phosphorus (BP) stands out from other 2D materials by the wide amplitude of the band-gap energy (Delta(Eg)) that sweeps an optical window from Visible (VIS) to Infrared (IR) wavelengths, depending on the layer thickness. This singularity made the optical and excitonic properties of BP difficult to map. Specifically, the literature lacks in presenting experimental and theoretical data on the optical properties of BP on an extended thickness range. Here we report the study of an ensemble of photoluminescence spectra from 79 passivated BP flakes recorded at 4 K with thicknesses ranging from 4 nm to 700 nm, obtained by mechanical exfoliation. We observe that the exfoliation steps induce additional defects states that compete the radiative recombination from bound excitons observed in the crystal. We also show that the evolution of the photoluminescence energy versus thickness follows a quantum well confinement model appreciable from a thickness predicted and probed at 25 nm. The BP slabs placed in different 2D heterostructures show that the emission energy is not significantly modulated by the dielectric environment. Introduction Confinement effects, Comment: 11 pages, 3 figures - Main text 12 pages, 5 figures - Supporting information

Superconducting proximity effects in graphene have received a great deal of attention for over a decade now. This has unveiled a plethora of exotic effects linked to the specificities of graphene's electronic properties. The vast majority of the related studies are based on conventional, low-temperature superconducting metals with isotropic $s$-wave pairing. Here we review recent advances made on the less studied case of unconventional high-temperature superconducting cuprates. These are characterized by an anisotropic $d$-wave pairing, whose interplay with Dirac electrons yields very rich physics and novel proximity behaviours. We provide a theoretical analysis and summarize the experiments reported so far. These unveil hints of proximity-induced unconventional pairing and demonstrate the gate-tunable, long-range propagation of high-temperature superconducting correlations in graphene. Finally, the fundamental and technological opportunities brought by the theoretical and experimental advances are discussed, together with the interest in extending similar studies to other Dirac materials., Comment: Short review on d-wave proximity in graphene and other 2D Dirac materials, 30 pages and 12 figures

Spintronic structures are extensively investigated for their spin orbit torque properties, required for magnetic commutation functionalities. Current progress in these materials is dependent on the interface engineering for the optimization of spin transmission. Here, we advance the analysis of ultrafast spin-charge conversion phenomena at ferromagnetic-transition metal interfaces due to their inverse spin-Hall effect properties. In particular the intrinsic inverse spin Hall effect of Pt-based systems and extrinsic inverse spin-Hall effect of Au:W and Au:Ta in NiFe/Au:(W,Ta) bilayers are investigated. The spin-charge conversion is probed by complementary techniques -- ultrafast THz time domain spectroscopy in the dynamic regime for THz pulse emission and ferromagnetic resonance spin-pumping measurements in the GHz regime in the steady state -- to determine the role played by the material properties, resistivities, spin transmission at metallic interfaces and spin-flip rates. These measurements show the correspondence between the THz time domain spectroscopy and ferromagnetic spin-pumping for the different set of samples in term of the spin mixing conductance. The latter quantity is a critical parameter, determining the strength of the THz emission from spintronic interfaces. This is further supported by ab-initio calculations, simulations and analysis of the spin-diffusion and spin relaxation of carriers within the multilayers in the time domain, permitting to determine the main trends and the role of spin transmission at interfaces. This work illustrates that time domain spectroscopy for spin-based THz emission is a powerful technique to probe spin-dynamics at active spintronic interfaces and to extract key material properties for spin-charge conversion., Comment: 20 pages

We report on the phosphonic acid route for the grafting of functional molecules, optical switch (dithienylethene diphosphonic acid, DDA), on La0.7Sr0.3MnO3 (LSMO). Compact self-assembled monolayers (SAMs) of DDA are formed on LSMO as studied by topographic atomic force microscopy (AFM), ellipsometry, water contact angle and X-ray photoemission spectroscopy (XPS). The conducting AFM measurements show that the electrical conductance of LSMO/DDA is about 3 decades below that of the bare LSMO substrate. Moreover, the presence of the DDA SAM suppresses the known conductance switching of the LSMO substrate that is induced by mechanical and/or bias constraints during C-AFM measurements. A partial light-induced conductance switching between the open and closed forms of the DDA is observed for the LSMO/DDA/C-AFM tip molecular junctions (closed/open conductance ratio of about 8). We show that, in the case of long-time exposition to UV light, this feature can be masked by a non-reversible decrease (a factor of about 15) of the conductance of the LSMO electrode., Comment: Full paper with supporting information

Recent experiments have shown that proximity with high-temperature superconductors induces unconventional superconducting correlations in graphene. Here we demonstrate that those correlations propagate hundreds of nanometer, allowing for the unique observation of $d$-wave Andreev pair interferences in YBa$_2$Cu$_3$O$_7$-graphene devices that behave as a Fabry-P\'erot cavity. The interferences show as a series of pronounced conductance oscillations analogous to those originally predicted by de Gennes--Saint-James for conventional metal-superconductor junctions. The present work is pivotal to the study of exotic directional effects expected for nodal superconductivity in Dirac materials., Comment: 4 pages with 4 figure

Superconductivity can be induced in a normal material via the leakage of superconducting pairs of charge carriers from an adjacent superconductor. This so-called proximity effect is markedly influenced by graphene unique electronic structure, both in fundamental and technologically relevant ways. These include an unconventional form of the leakage mechanism the Andreev reflection and the potential of supercurrent modulation through electrical gating. Despite the interest of high-temperature superconductors in that context, realizations have been exclusively based on low-temperature ones. Here we demonstrate gate-tunable, high-temperature superconducting proximity effect in graphene. Notably, gating effects result from the perfect transmission of superconducting pairs across an energy barrier -a form of Klein tunneling, up to now observed only for non-superconducting carriers- and quantum interferences controlled by graphene doping. Interestingly, we find that this type of interferences become dominant without the need of ultra-clean graphene, in stark contrast to the case of low-temperature superconductors. These results pave the way to a new class of tunable, high-temperature Josephson devices based on large-scale graphene.

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 at telecom wavelength, 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, $n_2 = - 1.1\times 10^{-13} m^2/W$. 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., Comment: To be published in Optics Letters

We report an optoelectronic mixer based on chemical vapour-deposited graphene. Our device consists in a coplanar waveguide that integrates a graphene channel, passivated with an atomic layer-deposited Al2O3 film. With this new structure, 30 GHz optoelectronic mixing in commercially-available graphene is demonstrated for the first time. In particular, using a 30 GHz intensity-modulated optical signal and a 29.9 GHz electrical signal, we show frequency downconversion to 100 MHz. These results open promising perspectives in the domain of optoelectronics for radar and radio-communication systems., Comment: 15 pages, 4 figures

Layered transition-metal dichalcogenides (TMDs) family are gaining increasing importance due to their unique electronic band structures, promising interplay among light, valley (pseudospin), charge and spin degrees of freedom. They possess large intrinsic spin-orbit interaction which make them most relevant for the emerging field of spin-orbitronics. Here we report on the conversion of spin current to charge current in MoS2 monolayer. Using spin pumping from a ferromagnetic layer (10 nm of cobalt) we find that the spin to charge conversion is highly efficient. Analysis in the frame of the inverse Rashba-Edelstein (RE) effect yields a RE length in excess of 4 nm at room temperature. Furthermore, owing to the semiconducting nature of MoS$_{2}$, it is found that back-gating allows electrical field control of the spin-relaxation rate of the MoS$_{2}$-metallic stack.

Because of its fascinating electronic properties, graphene is expected to produce breakthroughs in many areas of nanoelectronics. For spintronics, its key advantage is the expected long spin lifetime, combined with its large electron velocity. In this article, we review recent theoretical and experimental results showing that graphene could be the long-awaited platform for spintronics. A critical parameter for both characterization and devices is the resistance of the contact between the electrodes and the graphene, which must be large enough to prevent quenching of the induced spin polarization but small enough to allow for the detection of this polarization. Spin diffusion lengths in the 100-{\mu}m range, much longer than those in conventional metals and semiconductors, have been observed. This could be a unique advantage for several concepts of spintronic devices, particularly for the implementation of complex architectures or logic circuits in which information is coded by pure spin currents.

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 vapour deposition (CVD) process allows the preservation of an unoxidized nickel surface upon air exposure. Fabrication and measurement of complete reference tunneling spin valve structures demonstrates 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.

Spin information processing is a possible new paradigm for post-CMOS (complementary metal-oxide semiconductor) electronics and efficient spin propagation over long distances is fundamental to this vision. However, despite several decades of intense research, a suitable platform is still wanting. We report here on highly efficient spin transport in two-terminal polarizer/analyser devices based on high-mobility epitaxial graphene grown on silicon carbide. Taking advantage of high-impedance injecting/detecting tunnel junctions, we show spin transport efficiencies up to 75%, spin signals in the mega-ohm range and spin diffusion lengths exceeding 100 {\mu}m. This enables spintronics in complex structures: devices and network architectures relying on spin information processing, well beyond present spintronics applications, can now be foreseen.

The design of large-scale electronic circuits that are entirely spintronics-driven requires a current source that is highly spin-polarised at and beyond room temperature, cheap to build, efficient at the nanoscale and straightforward to integrate with semiconductors. Yet despite research within several subfields spanning nearly two decades, this key building block is still lacking. We experimentally and theoretically show how the interface between Co and phthalocyanine molecules constitutes a promising candidate. Spin-polarised direct and inverse photoemission experiments reveal a high degree of spin polarisation at room temperature at this interface. We measured a magnetic moment on the molecules's nitrogen pi orbitals, which substantiates an ab-initio theoretical description of highly spin-polarised charge conduction across the interface due to differing spinterface formation mechanims in each spin channel. We propose, through this example, a recipe to engineer simple organic-inorganic interfaces with remarkable spintronic properties that can endure well above room temperature.

We investigate the magneto-transport characteristics of nanospintronics single-electron devices. The devices consist of single non-magnetic nano-objects (nanometer size nanoparticles of Al or Cu) connected to Co ferromagnetic leads. The comparison with simulations allows us attribute the observed magnetoresistance to either spin accumulation or anisotropic magneto-Coulomb effect (AMC), two effects with very different origins. The fact that the two effects are observed in similar samples demonstrates that a careful analysis of Coulomb blockade and magnetoresistance behaviors is necessary in order to discriminate them in magnetic single-electron devices. As a tool for further studies, we propose a simple way to determine if spin transport or AMC effect dominates from the Coulomb blockade I-V curves of the spintronics device.

Whereas spintronics brings the spin degree of freedom to electronic devices, molecular/organic electronics adds the opportunity to play with the chemical versatility. Here we show how, as a contender to commonly used inorganic materials, organic/molecular based spintronics devices can exhibit very large magnetoresistance and lead to tailored spin polarizations. We report on giant tunnel magnetoresistance of up to 300% in a (La,Sr)MnO3/Alq3/Co nanometer size magnetic tunnel junction. Moreover, we propose a spin dependent transport model giving a new understanding of spin injection into organic materials/molecules. Our findings bring a new insight on how one could tune spin injection by molecular engineering and paves the way to chemical tailoring of the properties of spintronics devices., Comment: Original version. Revised version to appear in Nature Physics.

We have fabricated nanometer sized magnetic tunnel junctions using a new nanoindentation technique in order to study the transport properties of a single metallic nanoparticle. Coulomb blockade effects show clear evidence for single electron tunneling through a single 2.5 nm Au cluster. The observed magnetoresistance is the signature of spin conservation during the transport process through a non magnetic cluster., Comment: 3 pages

We report on the fabrication of nanocontacts by indentation of an ultrathin insulating photoresist layer deposited on various types of conductive structures. A modified atomic force microscope (AFM) designed for local resistance measurements is used as a nanoindenter. The nanoindentation is performed while measuring continuously the resistance between the conductive tip of the AFM and the conductive layer, which is used as the trigger parameter to stop the indentation. This allows an extremely accurate control of the indentation process. The indented hole is subsequently filled by a metal to create a contact on the underlying layer. We show that nanocontacts in the range of 1 to 10 nm2 can be created with this technique.

Quasiparticle tunneling spectra of the electron-doped (n-type) infinite-layer cuprate Sr_{0.9}La_{0.1}CuO_2 reveal characteristics that counter a number of common phenomena in the hole-doped (p-type) cuprates. The optimally doped Sr_{0.9}La_{0.1}CuO_2 with T_c = 43 K exhibits a momentum-independent superconducting gap \Delta = 13.0 +- 1.0 meV that substantially exceeds the BCS value, and the spectral characteristics indicate insignificant quasiparticle damping by spin fluctuations and the absence of pseudogap. The response to quantum impurities in the Cu-sites also differs fundamentally from that of the p-type cuprates with d_{x^2-y^2}-wave pairing symmetry., Comment: 4 pages, 3 figures. Published in Physical Review Letter. Corresponding author: Nai-Chang Yeh (e-mail: ncyeh@caltech.edu)

Scanning tunneling spectroscopy of superconducting MgB$_2$ ($T_c = 39$ K) were studied on high-density pellets and c-axis oriented films. The sample surfaces were chemically etched to remove surface carbonates and hydroxides, and the data were compared with calculated spectra for all symmetry-allowed pairing channels. The pairing potential ($\Delta_k$) is best described by an anisotropic s-wave pairing model, with $\Delta_k = \Delta_{xy} \sin ^2 \theta_k + \Delta_z \cos ^2 \theta_k$, where $\theta_k$ is the angle relative to the crystalline c-axis, $\Delta_z \sim 8.0$ meV, and $\Delta_{xy} \sim 5.0$ meV., Comment: 4 pages and 3 figures. Submitted to Physical Review Letters. Corresponding author: Nai-Chang Yeh (e-mail: ncyeh@caltech.edu)