Size-Dependence and High Temperature Stability of Radial Vortex Magnetic Textures Imprinted by Superconductor Stray Fields.

Swirling spin textures, including topologically nontrivial states, such as skyrmions, chiral domain walls, and magnetic vortices, have garnered significant attention within the scientific community due to their appeal from both fundamental and applied points of view. However, their creation, controlled manipulation, and stability are typically constrained to certain systems with specific crystallographic symmetries, bulk or interface interactions, and/or a precise stacking sequence of materials. Recently, a new approach has shown potential for the imprint of magnetic radial vortices in soft ferromagnetic compounds making use of the stray field of YBa2Cu3O7-δ superconducting microstructures in ferromagnet/superconductor (FM/SC) hybrids at temperatures below the superconducting transition temperature (TC). Here, we explore the lower size limit for the imprint of magnetic radial vortices in square and disc shaped structures as well as the persistence of these spin textures above TC, with magnetic domains retaining partial memory. Structures with circular geometry and with FM patterned to smaller radius than the superconductor island facilitate the imprinting of magnetic radial vortices and improve their stability above TC, in contrast to square structures where the presence of magnetic domains increases the dipolar energy. Micromagnetic modeling coupled with a SC field model reveals that the stabilization mechanism above TC is mediated by microstructural defects. Superconducting control of swirling spin textures, and their stabilization above the superconducting transition temperature by means of defect engineering holds promising prospects for shaping superconducting spintronics based on magnetic textures.

Bimodal ionic photomemristor based on a high-temperature oxide superconductor/semiconductor junction.

Memristors, a cornerstone for neuromorphic electronics, respond to the history of electrical stimuli by varying their electrical resistance across a continuum of states. Much effort has been recently devoted to developing an analogous response to optical excitation. Here we realize a novel tunnelling photo-memristor whose behaviour is bimodal: its resistance is determined by the dual electrical-optical history. This is obtained in a device of ultimate simplicity: an interface between a high-temperature superconductor and a transparent semiconductor. The exploited mechanism is a reversible nanoscale redox reaction between both materials, whose oxygen content determines the electron tunnelling rate across their interface. The redox reaction is optically driven via an interplay between electrochemistry, photovoltaic effects and photo-assisted ion migration. Besides their fundamental interest, the unveiled electro-optic memory effects have considerable technological potential. Especially in combination with high-temperature superconductivity which, in addition to facilitating low-dissipation connectivity, brings photo-memristive effects to the realm of superconducting electronics.

Almost Perfect Spin Filtering in Graphene-Based Magnetic Tunnel Junctions.

We report on large spin-filtering effects in epitaxial graphene-based spin valves, strongly enhanced in our specific multilayer case. Our results were obtained by the effective association of chemical vapor deposited (CVD) multilayer graphene with a high quality epitaxial Ni(111) ferromagnetic spin source. We highlight that the Ni(111) spin source electrode crystallinity and metallic state are preserved and stabilized by multilayer graphene CVD growth. Complete nanometric spin valve junctions are fabricated using a local probe indentation process, and spin properties are extracted from the graphene-protected ferromagnetic electrode through the use of a reference Al2O3/Co spin analyzer. Strikingly, spin-transport measurements in these structures give rise to large negative tunnel magneto-resistance TMR = -160%, pointing to a particularly large spin polarization for the Ni(111)/Gr interface PNi/Gr, evaluated up to -98%. We then discuss an emerging physical picture of graphene-ferromagnet systems, sustained both by experimental data and ab initio calculations, intimately combining efficient spin filtering effects arising (i) from the bulk band structure of the graphene layers purifying the extracted spin direction, (ii) from the hybridization effects modulating the amplitude of spin polarized scattering states over the first few graphene layers at the interface, and (iii) from the epitaxial interfacial matching of the graphene layers with the spin-polarized Ni surface selecting well-defined spin polarized channels. Importantly, these main spin selection effects are shown to be either cooperating or competing, explaining why our transport results were not observed before. Overall, this study unveils a path to harness the full potential of low Resitance.Area (RA) graphene interfaces in efficient spin-based devices.

Combined spin filtering actions in hybrid magnetic junctions based on organic chains covalently attached to graphene.

We present a bias-controlled spin-filtering mechanism in spin-valves including a hybrid organic chain/graphene interface. Wet growth conditions of oligomeric molecular chains would usually lead, during standard CMOS-compatible fabrication processes, to the quenching of spintronics properties of metallic spin sources due to oxidation. We demonstrate by X-ray photoelectron spectroscopy that the use of a protective graphene layer fully preserves the metallic character of the ferromagnetic surface and thus its capability to deliver spin polarized currents. We focus here on a small aromatic chain of controllable lengths, formed by nitrobenzene monomers and derived from the commercial 4-nitrobenzene diazonium tetrafluoroborate, covalently attached to the graphene passivated spin sources thanks to electroreduction. A unique bias dependent switch of the spin signal is then observed in complete spin valve devices, from minority to majority spin carriers filtering. First-principles calculations are used to highlight the key role played by the spin-dependent hybridization of electronic states present at the different interfaces. Our work is a first step towards the exploration of spin transport using different functional molecular chains. It opens the perspective of atomic tailoring of magnetic junction devices towards spin and quantum transport control, thanks to the flexibility of ambient electrochemical surface functionalization processes.

An Oxygen Vacancy Memristor Ruled by Electron Correlations.

Resistive switching effects offer new opportunities in the field of conventional memories as well as in the booming area of neuromorphic computing. Here the authors demonstrate memristive switching effects produced by a redox-driven oxygen exchange in tunnel junctions based on NdNiO3 , a strongly correlated electron system characterized by the presence of a metal-to-insulator transition (MIT). Strikingly, a strong interplay exists between the MIT and the redox mechanism, which on the one hand modifies the MIT itself, and on the other hand radically affects the tunnel resistance switching and the resistance states' lifetime. That results in a very unique temperature behavior and endows the junctions with multiple degrees of freedom. The obtained results bring up fundamental questions on the interplay between electronic correlations and the creation and mobility of oxygen vacancies in nickelates, opening a new avenue toward mimicking neuromorphic functions by exploiting the electric-field control of correlated states.

Spin-Charge Interconversion in KTaO3 2D Electron Gases.

Oxide interfaces exhibit a broad range of physical effects stemming from broken inversion symmetry. In particular, they can display non-reciprocal phenomena when time reversal symmetry is also broken, e.g., by the application of a magnetic field. Examples include the direct and inverse Edelstein effects (DEE, IEE) that allow the interconversion between spin currents and charge currents. The DEE and IEE have been investigated in interfaces based on the perovskite SrTiO3 (STO), albeit in separate studies focusing on one or the other. The demonstration of these effects remains mostly elusive in other oxide interface systems despite their blossoming in the last decade. Here, the observation of both the DEE and IEE in a new interfacial two-dimensional electron gas (2DEG) based on the perovskite oxide KTaO3 is reported. 2DEGs are generated by the simple deposition of Al metal onto KTaO3 single crystals, characterized by angle-resolved photoemission spectroscopy and magnetotransport, and shown to display the DEE through unidirectional magnetoresistance and the IEE by spin-pumping experiments. Their spin-charge interconversion efficiency is then compared with that of STO-based interfaces, related to the 2DEG electronic structure, and perspectives are given for the implementation of KTaO3 2DEGs into spin-orbitronic devices is compared.

Band-Gap Landscape Engineering in Large-Scale 2D Semiconductor van der Waals Heterostructures.

We present a growth process relying on pulsed laser deposition for the elaboration of complex van der Waals heterostructures on large scales, at a 400 °C CMOS-compatible temperature. Illustratively, we define a multilayer quantum well geometry through successive in situ growths, leading to WSe2 being encapsulated into WS2 layers. The structural constitution of the quantum well geometry is confirmed by Raman spectroscopy combined with transmission electron microscopy. The large-scale high homogeneity of the resulting 2D van der Waals heterostructure is also validated by macro- and microscale Raman mappings. We illustrate the benefit of this integrative in situ approach by showing the structural preservation of even the most fragile 2D layers once encapsulated in a van der Waals heterostructure. Finally, we fabricate a vertical tunneling device based on these large-scale layers and discuss the clear signature of electronic transport controlled by the quantum well configuration with ab initio calculations in support. The flexibility of this direct growth approach, with multilayer stacks being built in a single run, allows for the definition of complex 2D heterostructures barely accessible with usual exfoliation or transfer techniques of 2D materials. Reminiscent of the III-V semiconductors' successful exploitation, our approach unlocks virtually infinite combinations of large 2D material families in any complex van der Waals heterostructure design.

Mapping spin-charge conversion to the band structure in a topological oxide two-dimensional electron gas.

While spintronics has traditionally relied on ferromagnetic metals as spin generators and detectors, spin-orbitronics exploits the efficient spin-charge interconversion enabled by spin-orbit coupling in non-magnetic systems. Although the Rashba picture of split parabolic bands is often used to interpret such experiments, it fails to explain the largest conversion effects and their relationship with the electronic structure. Here, we demonstrate a very large spin-to-charge conversion effect in an interface-engineered, high-carrier-density SrTiO3 two-dimensional electron gas and map its gate dependence on the band structure. We show that the conversion process is amplified by enhanced Rashba-like splitting due to orbital mixing and in the vicinity of avoided band crossings with topologically non-trivial order. Our results indicate that oxide two-dimensional electron gases are strong candidates for spin-based information readout in new memory and transistor designs. Our results also emphasize the promise of topology as a new ingredient to expand the scope of complex oxides for spintronics.

Growth and Electrostatic/chemical Properties of Metal/LaAlO3/SrTiO3 Heterostructures.

The quasi 2D electron system (q2DES) that forms at the interface between LaAlO3 (LAO) and SrTiO3 (STO) has attracted much attention from the oxide electronics community. One of its hallmark features is the existence of a critical LAO thickness of 4 unit-cells (uc) for interfacial conductivity to emerge. Although electrostatic mechanisms have been proposed in the past to describe the existence of this critical thickness, the importance of chemical defects has been recently accentuated. Here, we describe the growth of metal/LAO/STO heterostructures in an ultra-high vacuum (UHV) cluster system combining pulsed laser deposition (to grow the LAO), magnetron sputtering (to grow the metal) and X-ray photoelectron spectroscopy (XPS). We study step by step the formation and evolution of the q2DES and the chemical interactions that occur between the metal and the LAO/STO. Additionally, magnetotransport experiments elucidate on the transport and electronic properties of the q2DES. This systematic work not only demonstrates a way to study the electrostatic and chemical interplay between the q2DES and its environment, but also unlocks the possibility to couple multifunctional capping layers with the rich physics observed in two-dimensional electron systems, allowing the fabrication of new types of devices.

Tuning Up or Down the Critical Thickness in LaAlO3 /SrTiO3 through In Situ Deposition of Metal Overlayers.

The quasi 2D electron system (q2DES) that forms at the interface between LaAlO3 and SrTiO3 has attracted much attention from the oxide electronics community. One of its hallmark features is the existence of a critical LaAlO3 thickness of 4 unit-cells (uc) for interfacial conductivity to emerge. In this paper, the chemical, electronic, and transport properties of LaAlO3 /SrTiO3 samples capped with different metals grown in a system combining pulsed laser deposition, sputtering, and in situ X-ray photoemission spectroscopy are investigated. The results show that for metals with low work function a q2DES forms at 1-2 uc of LaAlO3 and is accompanied by a partial oxidation of the metal, a phenomenon that affects the q2DES properties and triggers the formation of defects. In contrast, for noble metals, the critical thickness is increased above 4 uc. The results are discussed in terms of a hybrid mechanism that incorporates electrostatic and chemical effects.

Thermally and photoinduced polymerization of ultrathin sexithiophene films.

The thermally-induced polymerization of α-sexithiophene (6T) molecules on Ag(001) and Au(001) gives rise to long unbranched polymer chains or branched polymer networks depending on the annealing parameters. There, the onset temperature for polymerization depends on the strength of interaction with the underlying substrate. Similar polymerization processes are also induced by ultraviolet radiation with photon energies between 3.0 and 4.2 eV. Radical formation by an electronic excitation in the 6T molecule is proposed as the driving mechanism that necessitates the interplay with the metallic substrate.