Hicham Majjad

Nanotrench for nano and microparticle electrical interconnects

We present a simple and versatile patterning procedure for the reliable and reproducible fabrication of high aspect ratio (10(4)) electrical interconnects that have separation distances down to 20 nm and lengths of several hundreds of microns. The process uses standard optical lithography techniques and allows parallel processing of many junctions, making it easily scalable and industrially relevant. We demonstrate the suitability of these nanotrenches as electrical interconnects for addressing micro and nanoparticles by realizing several circuits with integrated species. Furthermore, low impedance metal-metal low contacts are shown to be obtained when trapping a single metal-coated microsphere in the gap, emphasizing the intrinsic good electrical conductivity of the interconnects, even though a wet process is used. Highly resistive magnetite-based nanoparticles networks also demonstrate the advantage of the high aspect ratio of the nanotrenches for providing access to electrical properties of highly resistive materials, with leakage current levels below 1 pA.

Electrical switching in Fe∕Cr∕MgO∕Fe magnetic tunnel junctions

Hysteretic resistance switching is observed in epitaxial Fe∕Cr∕MgO∕Fe magnetic tunnel junctions under bias voltage cycling between negative and positive values of about 1V. The junctions switch back and forth between high- and low-resistance states, both of which depend on the device bias history. A linear dependence is found between the magnitude of the tunnel magnetoresistance and the crafted resistance of the junctions. To explain these results, a model is proposed that considers electron transport both by elastic tunneling and by defect-assisted transmission.

Localized states in advanced dielectrics from the vantage of spin- and symmetry-polarized tunnelling across MgO

Research on advanced materials such as multiferroic perovskites underscores promising applications, yet studies on these materials rarely address the impact of defects on the nominally expected materials property. Here, we revisit the comparatively simple oxide MgO as the model material system for spin-polarized solid-state tunnelling studies. We present a defect-mediated tunnelling potential landscape of localized states owing to explicitly identified defect species, against which we examine the bias and temperature dependence of magnetotransport. By mixing symmetry-resolved transport channels, a localized state may alter the effective barrier height for symmetry-resolved charge carriers, such that tunnelling magnetoresistance decreases most with increasing temperature when that state is addressed electrically. Thermal excitation promotes an occupancy switchover from the ground to the excited state of a defect, which impacts these magnetotransport characteristics. We thus resolve contradictions between experiment and theory in this otherwise canonical spintronics system, and propose a new perspective on defects in dielectrics.

Size-induced enhanced magnetoelectric effect and multiferroicity in chromium oxide nanoclusters

The control of the magnetization of a material with an electric field would make the design and the integration of novel electronic devices possible. This explains the renewed interest in multiferroic materials. Progress in this field is currently hampered by the scarcity of the materials available and the smallness of the magnetoelectric effects. Here we present a proof-of-principle experiment showing that engineering large strains through nanoscale size reduction is an efficient route for increasing magnetoelectric coefficients by orders of magnitude. The archetype magnetoelectric material, Cr2O3, in the form of epitaxial clusters, exhibits an unprecedented 600% change in magnetization magnitude under 1 V. Furthermore, a multiferroic phase, with both magnetic and electric spontaneous polarizations, is found in the clusters, while absent in the bulk.

Sub-coercive and multi-level ferroelastic remnant states with resistive readout

Ferroelectric devices use their electric polarization ferroic order as the switching and storage physical quantity for memory applications. However, additional built-in physical quantities and memory paradigms are requested for applications. We propose here to take advantage of the multiferroic properties of ferroelectrics, using ferroelasticity to create a remnant strain, persisting after stressing the material by converse piezoelectricity means. While large electric fields are needed to switch the polarization, here writing occurs at subcoercive much lower field values, which can efficiently imprint multiple remnant strain states. A proof-of-principle cell, with the simplest and non-optimized resistance strain detection design, is shown here to exhibit 13-memory states of high reproducibility and reliability. The related advantages in lower power consumption and limited device fatigue make our approach relevant for applications.

Photoinduced Cross-Linking of Dynamic Poly(disulfide) Films via Thiol Oxidative Coupling.

Initially developed as an elastomer with an excellent record of barrier and chemical resistance properties, poly(disulfide) has experienced a revival linked to the dynamic nature of the S-S covalent bond. A novel photobase-catalyzed oxidative polymerization of multifunctional thiols to poly(disulfide) network is reported. Based solely on air oxidation, the single-step process is triggered by the photodecarboxylation of a xanthone acetic acid liberating a strong bicyclic guanidine base. Starting with a 1 μm thick film based on trithiol poly(ethylene oxide) oligomer, the UV-mediated oxidation of thiols to disulfides occurs in a matter of minutes both selectively, i.e., without overoxidation, and quantitatively as assessed by a range of spectroscopic techniques. Thiolate formation and film thickness determine the reaction rates and yield. Spatial control of the photopolymerization serves to generate robust micropatterns, while the reductive cleavage of S-S bridges allows the recycling of 40% of the initial thiol groups.

Epitaxy of MgO magnetic tunnel barriers on epitaxial graphene

Epitaxial growth of electrodes and tunnel barriers on graphene is one of the main technological bottlenecks for graphene spintronics. In this paper, we demonstrate that MgO(111) epitaxial tunnel barriers, one of the prime candidates for spintronic application, can be grown by molecular beam epitaxy on epitaxial graphene on SiC(0001). Ferromagnetic metals (Fe, Co, Fe20Ni80) were epitaxially grown on top of the MgO barrier, thus leading to monocrystalline electrodes on graphene. Structural and magnetic characterizations were performed on these ferromagnetic metals after annealing and dewetting: they form clusters with a 100 nm typical lateral width, which are mostly magnetic monodomains in the case of Fe. This epitaxial stack opens the way to graphene spintronic devices taking benefits from a coherent tunnelling current through the epitaxial MgO/graphene stack.

Random barrier double-well model for resistive switching in tunnel barriers

The resistive switching phenomenon in MgO-based tunnel junctions is attributed to the effect of charged defects inside the barrier. The presence of electron traps in the MgO barrier, which can be filled and emptied, locally modifies the conductance of the barrier and leads to the resistive switching effects. A double-well model for trapped electrons in MgO is introduced to theoretically describe this phenomenon. Including the statistical distribution of potential barrier heights for these traps leads to a power-law dependence of the resistance as a function of time, under a constant bias voltage. This model also predicts a power-law relation of the hysteresis as a function of the voltage sweep frequency. Experimental transport results strongly support this model and in particular confirm the expected power laws dependencies of resistance. They moreover indicate that the exponent of these power laws varies with temperature as theoretically predicted.

The magnetoelectrochemical switch

Significance The magnetic gradient force field offers numerous possibilities to position and manipulate magnetic nanoparticles, but has limited influence on paramagnetic molecules in solutions. We argue here that proper design and miniaturization of ferromagnetic electrodes create huge force fields in their vicinity, tunable by an external magnetic field. We illustrate this concept by presenting how the conduction of a Ni metallic nanobridge is drastically modified by the Ni redox reactions equilibrium shifted under magnetic control, creating the chemical equivalent of the solid-state spin valve device. While the importance of the magnetic field amplitude on chemical reactions is well documented, our findings suggest that the magnetic field gradient can become a dominant influencing factor on chemical reactions at the nanoscale. In the field of spintronics, the archetype solid-state two-terminal device is the spin valve, where the resistance is controlled by the magnetization configuration. We show here how this concept of spin-dependent switch can be extended to magnetic electrodes in solution, by magnetic control of their chemical environment. Appropriate nanoscale design allows a huge enhancement of the magnetic force field experienced by paramagnetic molecular species in solutions, which changes between repulsive and attractive on changing the electrodes’ magnetic orientations. Specifically, the field gradient force created within a sub-100-nm-sized nanogap separating two magnetic electrodes can be reversed by changing the orientation of the electrodes’ magnetization relative to the current flowing between the electrodes. This can result in a breaking or making of an electric nanocontact, with a change of resistance by a factor of up to 103. The results reveal how an external field can impact chemical equilibrium in the vicinity of nanoscale magnetic circuits.

Oxygen-vacancy driven tunnelling spintronics across MgO

The conservation of an electron’s spin and symmetry as it undergoes solid-state tunnelling within magnetic tunnel junctions (MTJs) is thought to be best understood using MgO-based MTJs1. Yet the very large experimental values of tunnelling magnetoresistance (TMR) that justify this perception are often associated with tunnelling barrier heights well below those suggested by the MgO optical band gap. This combination of high TMR and low RA-product, while spawning spin-transfer/spin-orbit torque experiments and considerable industrial interest, cannot be explained by standard theory. Noting the impact of a tunnel barrier’s altered stoichiometry on TMR2, we reconcile this 10+year-old contradiction between theory and experiment by considering the impact of the MgO barrier’s structural defects3–5. We find that the ground and excited states of oxygen vacancies can promote localized states within the band gap with differing electronic character. By setting symmetry- and temperature-dependent tunnelling barrier heights, they alter symmetry-polarized tunnelling and thus TMR. We will examine how annealing, depending on MgO growth conditions, can alter the nature of these localized states. This oxygen vacancy paradigm of inorganic tunnelling spintronics opens interesting perspectives into endowing the MTJ with additional functionalities, such as optically manipulating the MTJ’s spintronic response.