Voltage-based magnetization switching and reading in magnetoelectric spin-orbit nanodevices.

As CMOS technologies face challenges in dimensional and voltage scaling, the demand for novel logic devices has never been greater, with spin-based devices offering scaling potential, at the cost of significantly high switching energies. Alternatively, magnetoelectric materials are predicted to enable low-power magnetization control, a solution with limited device-level results. Here, we demonstrate voltage-based magnetization switching and reading in nanodevices at room temperature, enabled by exchange coupling between multiferroic BiFeO3 and ferromagnetic CoFe, for writing, and spin-to-charge current conversion between CoFe and Pt, for reading. We show that, upon the electrical switching of the BiFeO3, the magnetization of the CoFe can be reversed, giving rise to different voltage outputs. Through additional microscopy techniques, magnetization reversal is linked with the polarization state and antiferromagnetic cycloid propagation direction in the BiFeO3. This study constitutes the building block for magnetoelectric spin-orbit logic, opening a new avenue for low-power beyond-CMOS technologies.

Toward sub-second solution exchange dynamics in flow reactors for liquid-phase transmission electron microscopy.

Liquid-phase transmission electron microscopy is a burgeoning experimental technique for monitoring nanoscale dynamics in a liquid environment, increasingly employing microfluidic reactors to control the composition of the sample solution. Current challenges comprise fast mass transport dynamics inside the central nanochannel of the liquid cell, typically flow cells, and reliable fixation of the specimen in the limited imaging area. In this work, we present a liquid cell concept - the diffusion cell - that satisfies these seemingly contradictory requirements by providing additional on-chip bypasses to allow high convective transport around the nanochannel in which diffusive transport predominates. Diffusion cell prototypes are developed using numerical mass transport models and fabricated on the basis of existing two-chip setups. Important hydrodynamic parameters, i.e., the total flow resistance, the flow velocity in the imaging area, and the time constants of mixing, are improved by 2-3 orders of magnitude compared to existing setups. The solution replacement dynamics achieved within seconds already match the mixing timescales of many ex-situ scenarios, and further improvements are possible. Diffusion cells can be easily integrated into existing liquid-phase transmission electron microscopy workflows, provide correlation of results with ex-situ experiments, and can create additional research directions addressing fast nanoscale processes.

Odd Nonlinear Conductivity under Spatial Inversion in Chiral Tellurium.

Electrical transport in noncentrosymmetric materials departs from the well-established phenomenological Ohm's law. Instead of a linear relation between current and electric field, a nonlinear conductivity emerges along specific crystallographic directions. This nonlinear transport is fundamentally related to the lack of spatial inversion symmetry. However, the experimental implications of an inversion symmetry operation on the nonlinear conductivity remain to be explored. Here, we report on a large, nonlinear conductivity in chiral tellurium. By measuring samples with opposite handedness, we demonstrate that the nonlinear transport is odd under spatial inversion. Furthermore, by applying an electrostatic gate, we modulate the nonlinear output by a factor of 300, reaching the highest reported value excluding engineered heterostructures. Our results establish chiral tellurium as an ideal compound not just to study the fundamental interplay between crystal structure, symmetry operations and nonlinear transport; but also to develop wireless rectifiers and energy-harvesting chiral devices.

Thermal Stability of Cu-Al-Ni Shape Memory Alloy Thin Films Obtained by Nanometer Multilayer Deposition.

Cu-Al-Ni is a high-temperature shape memory alloy (HTSMA) with exceptional thermomechanical properties, making it an ideal active material for engineering new technologies able to operate at temperatures up to 200 °C. Recent studies revealed that these alloys exhibit a robust superelastic behavior at the nanometer scale, making them excellent candidates for developing a new generation of micro-/nano-electromechanical systems (MEMS/NEMS). The very large-scale integration (VLSI) technologies used in microelectronics are based on thin films. In the present work, 1 µm thickness thin films of 84.1Cu-12.4 Al-3.5Ni (wt.%) were obtained by solid-state diffusion from a multilayer system deposited on SiNx (200 nm)/Si substrates by e-beam evaporation. With the aim of evaluating the thermal stability of such HTSMA thin films, heating experiments were performed in situ inside the transmission electron microscope to identify the temperature at which the material was decomposed by precipitation. Their microstructure, compositional analysis, and phase identification were characterized by scanning and transmission electron microscopy equipped with energy dispersive X-ray spectrometers. The nucleation and growth of two stable phases, Cu-Al-rich alpha phase and Ni-Al-rich intermetallic, were identified during in situ heating TEM experiments between 280 and 450 °C. These findings show that the used production method produces an HTSMA with high thermal stability and paves the road for developing high-temperature MEMS/NEMS using shape memory and superelastic technologies.

Quantification of reagent mixing in liquid flow cells for Liquid Phase-TEM.

Liquid-Phase Transmission Electron Microscopy (LP-TEM) offers the opportunity to study nanoscale dynamics of phenomena related to materials and life science in a native liquid environment and in real time. Until now, the opportunity to control/induce such dynamics by changing the chemical environment in the liquid flow cell (LFC) has rarely been exploited due to an incomplete understanding of hydrodynamic properties of LP-TEM flow systems. This manuscript introduces a method for hydrodynamic characterization of LP-TEM flow systems based on monitoring transmitted intensity while flowing a strongly electron scattering contrast agent solution. Key characteristic temporal indicators of solution replacement for various channel geometries were experimentally measured. A numerical physical model of solute transport based on realistic flow channel geometries was successfully implemented and validated against experiments. The model confirmed the impact of flow channel geometry on the importance of convective and diffusive solute transport, deduced by experiment, and could further extend understanding of hydrodynamics in LP-TEM flow systems. We emphasize that our approach can be applied to hydrodynamic characterization of any customized LP-TEM flow system. We foresee the implemented predictive model driving the future design of application-specific LP-TEM flow systems and, when combined with existing chemical reaction models, to a flourishing of the planning and interpretation of experimental observations.

All-Electrical Spin-to-Charge Conversion in Sputtered BixSe1-x.

One of the major obstacles to realizing spintronic devices such as MESO logic devices is the small signal magnitude used for magnetization readout, making it important to find materials with high spin-to-charge conversion efficiency. Although intermixing at the junction of two materials is a widely occurring phenomenon, its influence on material characterization and the estimation of spin-to-charge conversion efficiencies are easily neglected or underestimated. Here, we demonstrate all-electrical spin-to-charge conversion in BixSe1-x nanodevices and show how the conversion efficiency can be overestimated by tens of times depending on the adjacent metal used as a contact. We attribute this to the intermixing-induced compositional change and the properties of a polycrystal that lead to drastic changes in resistivity and spin Hall angle. Strategies to improve the spin-to-charge conversion signal in similar structures for functional devices are discussed.

Doping of Carbon Nanotubes with Encapsulated Phosphorus Chains.

Single-walled carbon nanotubes (SWCNTs) are a perfect host for the formation of one-dimensional phosphorus structures and to obtain hybrid materials with a large P-C ratio. This work presents a procedure for high-yield phosphorus filling of commercial Tuball SWCNTs and efficient removal of phosphorus deposits from the external nanotube surface. We probed white and red phosphorus as precursors, varied the synthesis temperature and the ampoule shape, and tested three solvents for sample purification. High-resolution transmission electron microscopy and Raman spectroscopy indicated crystallization of interior phosphorus in a form resembling fibrous red phosphorus. An aqueous sodium hydroxide solution allowed removing the majority of external phosphorus particles. Thermogravimetric analysis of the product determined ∼23 wt % (∼10 atom %) of phosphorus, and the X-ray photoelectron spectroscopy (XPS) data showed that ca. 80% of it is in the form of elemental phosphorus. Externally purified SWCNTs filled with phosphorus were used to study the interaction between the components. Raman spectroscopy and core-level XPS revealed p-type SWCNT doping. Valence-band XPS data and density functional theory calculations confirmed the transfer of the SWCNT electron density to the encapsulated phosphorus.

Gate-tuneable and chirality-dependent charge-to-spin conversion in tellurium nanowires.

Chiral materials are an ideal playground for exploring the relation between symmetry, relativistic effects and electronic transport. For instance, chiral organic molecules have been intensively studied to electrically generate spin-polarized currents in the last decade, but their poor electronic conductivity limits their potential for applications. Conversely, chiral inorganic materials such as tellurium have excellent electrical conductivity, but their potential for enabling the electrical control of spin polarization in devices remains unclear. Here, we demonstrate the all-electrical generation, manipulation and detection of spin polarization in chiral single-crystalline tellurium nanowires. By recording a large (up to 7%) and chirality-dependent unidirectional magnetoresistance, we show that the orientation of the electrically generated spin polarization is determined by the nanowire handedness and uniquely follows the current direction, while its magnitude can be manipulated by an electrostatic gate. Our results pave the way for the development of magnet-free chirality-based spintronic devices.

Double-Lattice Packing of Pentagonal Gold Bipyramids in Supercrystals with Triclinic Symmetry.

Pentagonal packing is a long-standing issue and a rich mathematical topic, brought to the fore by recent progress in nanoparticle design. Gold pentagonal bipyramids combine fivefold symmetry and anisotropy and their section varies along the length. In this work, colloidal supercrystals of pentagonal gold bipyramids are obtained in a compact arrangement that generalizes the optimal packing of regular pentagons in the plane. Multimodal investigations reveal a two-particle unit cell with triclinic symmetry, a lower symmetry than that of the building blocks. Monte Carlo computer simulations show that this lattice achieves the densest possible packing. Going beyond pentagons, further simulations show an odd-even effect of the number of sides on the packing: odd-sided bipyramids are non-centrosymmetric and require the double-lattice arrangement to recover inversion symmetry. The supercrystals display a facet-dependent optical response that is promising for sensing, metamaterials applications, and for fundamental studies of self-assembly processes.

Exchange Bias in Molecule/Fe3 GeTe2 van der Waals Heterostructures via Spinterface Effects.

The exfoliation of layered magnetic materials generates atomically thin flakes characterized by an ultrahigh surface sensitivity, which makes their magnetic properties tunable via external stimuli, such as electrostatic gating and proximity effects. Another powerful approach to engineer magnetic materials is molecular functionalization, generating hybrid interfaces with tailored magnetic interactions, called spinterfaces. However, spinterface effects have not yet been explored on layered magnetic materials. Here, the emergence of spinterface effects is demonstrated at the interface between flakes of the prototypical layered magnetic metal Fe3 GeTe2 and thin films of Co-phthalocyanine. Magnetotransport measurements show that the molecular layer induces a magnetic exchange bias in Fe3 GeTe2 , indicating that the unpaired spins in Co-phthalocyanine develop antiferromagnetic ordering and pin the magnetization reversal of Fe3 GeTe2 via magnetic proximity. The effect is strongest for a Fe3 GeTe2 thickness of 20 nm, for which the exchange bias field reaches -840 Oe at 10 K and is measurable up to ≈110 K. This value compares very favorably with previous exchange bias fields reported for Fe3 GeTe2 in all-inorganic van der Waals heterostructures, demonstrating the potential of molecular functionalization to tailor the magnetism of van der Waals layered materials.

Spin Hall Magnetoresistance Effect from a Disordered Interface.

The spin Hall magnetoresistance (SMR) emerged as a reference tool to investigate the magnetic properties of materials with an all-electrical setup. Its sensitivity to the magnetization of thin films and surfaces may turn it into a valuable technique to characterize van der Waals magnetic materials, which support long-range magnetic order in atomically thin layers. However, realistic surfaces can be affected by defects and disorder, which may result in unexpected artifacts in the SMR, rather than the sole appearance of electrical noise. Here, we study the SMR response of heterostructures combining a platinum (Pt) thin film with the van der Waals antiferromagnet MnPSe3 and observe a robust SMR-like signal, which turns out to originate from the presence of strong interfacial disorder in the system. We use transmission electron microscopy (TEM) to characterize the interface between MnPSe3 and Pt, revealing the formation of a few nanometer-thick platinum-chalcogen amorphous layer. The analysis of the transport and TEM measurements suggests that the signal arises from a disordered magnetic system formed at the Pt/MnPSe3 interface, washing out the interaction between the spins of the Pt electrons and the MnPSe3 magnetic lattice. Our results show that the damaged interfaces can yield an important contribution to SMR, questioning a widespread assumption on the role of disorder in such measurements.

Single-Walled Carbon Nanotubes with Red Phosphorus in Lithium-Ion Batteries: Effect of Surface and Encapsulated Phosphorus.

Single-walled carbon nanotubes (SWCNTs) with their high surface area, electrical conductivity, mechanical strength and elasticity are an ideal component for the development of composite electrode materials for batteries. Red phosphorus has a very high theoretical capacity with respect to lithium, but has poor conductivity and expends considerably as a result of the reaction with lithium ions. In this work, we compare the electrochemical performance of commercial SWCNTs with red phosphorus deposited on the outer surface of nanotubes and/or encapsulated in internal channels of nanotubes in lithium-ion batteries. External phosphorus, condensed from vapors, is easily oxidized upon contact with the environment and only the un-oxidized phosphorus cores participate in electrochemical reactions. The support of the SWCNT network ensures a stable long-term cycling for these phosphorus particles. The tubular space inside the SWCNTs stimulate the formation of chain phosphorus structures. The chains reversibly interact with lithium ions and provide a specific capacity of 1545 mAh·g-1 (calculated on the mass of phosphorus in the sample) at a current density of 0.1 A·g-1. As compared to the sample containing external phosphorus, SWCNTs with encapsulated phosphorus demonstrate higher reaction rates and a slight loss of initial capacity (~7%) on the 1000th cycle at 5 A·g-1.

Coupling plasmonic catalysis and nanocrystal growth through cyclic regeneration of NADH.

In a typical colloidal synthesis, the molecules of the reducing agent are irreversibly oxidized during nanocrystal growth. Such a scenario is of questionable sustainability when confronted with naturally occurring processes in which reducing agent molecules are cyclically regenerated. Here we show that cofactor molecules once consumed in the nucleation and growth of metallic nanocrystals can be photoregenerated using metallic nanocrystals as photocatalysts and reused in the subsequent nucleation process. Cyclic regeneration of cofactor molecules opens up the possibilities for the sustainable synthesis of inorganic nanoparticles.

In-SEM micro-machining reveals the origins of the size effect in the cutting energy.

High-precision metal cutting is increasingly relevant in advanced applications. Such precision normally requires a cutting feed in the micron or even sub-micron dimension scale, which raises questions about applicability of concepts developed in industrial scale machining. To address this challenge, we have developed a device to perform linear cutting with force measurement in the vacuum chamber of an electron microscope, which has been utilised to study the cutting process down to 200 nm of the feed and the tool tip radius. The machining experiments carried out in-operando in SEM have shown that the main classical deformation zones of metal cutting: primary, secondary and tertiary shear zones-were preserved even at sub-micron feeds. In-operando observations and subsequent structural analysis in FIB/SEM revealed a number of microstructural peculiarities, such as: a substantial increase of the cutting force related to the development of the primary shear zone; dependence of the ternary shear zone thickness on the underlaying grain crystal orientation. Measurement of the cutting forces at deep submicron feeds and cutting tool apex radii has been exploited to discriminate different sources for the size effect on the cutting energy (dependence of the energy on the feed and tool radius). It was observed that typical industrial values of feed and tool radius imposes a size effect determined primarily by geometrical factors, while in a sub-micrometre feed range the contribution of the strain hardening in the primary share zone becomes relevant.

Black Au-Decorated TiO2 Produced via Laser Ablation in Liquid.

The rational combination of plasmonic and all-dielectric concepts within hybrid nanomaterials provides a promising route toward devices with ultimate performance and extended modalities. Spectral matching of plasmonic and Mie-type resonances for such nanostructures can only be achieved for their dissimilar characteristic sizes, thus making the resulting hybrid nanostructure geometry complex for practical realization and large-scale replication. Here, we produced amorphous TiO2 nanospheres decorated and doped with Au nanoclusters via single-step nanosecond-laser irradiation of commercially available TiO2 nanopowders dispersed in aqueous HAuCl4. Fabricated hybrids demonstrate remarkable light-absorbing properties (averaged value ≈96%) in the visible and near-IR spectral range mediated by bandgap reduction of the laser-processed amorphous TiO2 as well as plasmon resonances of the decorating Au nanoclusters. The findings are supported by optical spectroscopy, electron energy loss spectroscopy, transmission electron microscopy, and electromagnetic modeling. Light-absorbing and plasmonic properties of the produced hybrids were implemented to demonstrate catalytically passive SERS biosensor for identification of analytes at trace concentrations and solar steam generator that permitted to increase water evaporation rate by 2.5 times compared with that of pure water under identical 1 sun irradiation conditions.

Strong Interfacial Exchange Field in a Heavy Metal/Ferromagnetic Insulator System Determined by Spin Hall Magnetoresistance.

Spin-dependent transport at heavy metal/magnetic insulator interfaces is at the origin of many phenomena at the forefront of spintronics research. A proper quantification of the different interfacial spin conductances is crucial for many applications. Here, we report the first measurement of the spin Hall magnetoresistance (SMR) of Pt on a purely ferromagnetic insulator (EuS). We perform SMR measurements in a wide range of temperatures and fit the results by using a microscopic model. From this fitting procedure, we obtain the temperature dependence of the spin conductances (Gs, Gr, and Gi), disentangling the contribution of field-like torque (Gi), damping-like torque (Gr), and spin-flip scattering (Gs). An interfacial exchange field of the order of 1 meV acting upon the conduction electrons of Pt can be estimated from Gi, which is at least three times larger than Gr below the Curie temperature. Our work provides an easy method to quantify this interfacial spin-splitting field, which plays a key role in emerging fields such as superconducting spintronics and caloritronics as well as topological quantum computation.

Magnetic Vortex Nanodiscs Enable Remote Magnetomechanical Neural Stimulation.

Magnetic nanomaterials in magnetic fields can serve as versatile transducers for remote interrogation of cell functions. In this study, we leveraged the transition from vortex to in-plane magnetization in iron oxide nanodiscs to modulate the activity of mechanosensory cells. When a vortex configuration of spins is present in magnetic nanomaterials, it enables rapid control over their magnetization direction and magnitude. The vortex configuration manifests in near zero net magnetic moment in the absence of a magnetic field, affording greater colloidal stability of magnetic nanomaterials in suspensions. Together, these properties invite the application of magnetic vortex particles as transducers of externally applied minimally invasive magnetic stimuli in biological systems. Using magnetic modeling and electron holography, we predict and experimentally demonstrate magnetic vortex states in an array of colloidally synthesized magnetite nanodiscs 98-226 nm in diameter. The magnetic nanodiscs applied as transducers of torque for remote control of mechanosensory neurons demonstrated the ability to trigger Ca2+ influx in weak (≤28 mT), slowly varying (≤5 Hz) magnetic fields. The extent of cellular response was determined by the magnetic nanodisc volume and magnetic field conditions. Magnetomechanical activation of a mechanosensitive cation channel TRPV4 (transient receptor potential vanilloid family member 4) exogenously expressed in the nonmechanosensitive HEK293 cells corroborated that the stimulation is mediated by mechanosensitive ion channels. With their large magnetic torques and colloidal stability, magnetic vortex particles may facilitate basic studies of mechanoreception and its applications to control electroactive cells with remote magnetic stimuli.

Enhanced magnetic modulation of light polarization exploiting hybridization with multipolar dark plasmons in magnetoplasmonic nanocavities.

Enhancing magneto-optical effects is crucial for reducing the size of key photonic devices based on the non-reciprocal propagation of light and to enable active nanophotonics. Here, we disclose a currently unexplored approach that exploits hybridization with multipolar dark modes in specially designed magnetoplasmonic nanocavities to achieve a large enhancement of the magneto-optically induced modulation of light polarization. The broken geometrical symmetry of the design enables coupling with free-space light and hybridization of the multipolar dark modes of a plasmonic ring nanoresonator with the dipolar localized plasmon resonance of the ferromagnetic disk placed inside the ring. This hybridization results in a low-radiant multipolar Fano resonance that drives a strongly enhanced magneto-optically induced localized plasmon. The large amplification of the magneto-optical response of the nanocavity is the result of the large magneto-optically induced change in light polarization produced by the strongly enhanced radiant magneto-optical dipole, which is achieved by avoiding the simultaneous enhancement of re-emitted light with incident polarization by the multipolar Fano resonance. The partial compensation of the magneto-optically induced polarization change caused by the large re-emission of light with the original polarization is a critical limitation of the magnetoplasmonic designs explored thus far and that is overcome by the approach proposed here.

Large Multidirectional Spin-to-Charge Conversion in Low-Symmetry Semimetal MoTe2 at Room Temperature.

Efficient and versatile spin-to-charge current conversion is crucial for the development of spintronic applications, which strongly rely on the ability to electrically generate and detect spin currents. In this context, the spin Hall effect has been widely studied in heavy metals with strong spin-orbit coupling. While the high crystal symmetry in these materials limits the conversion to the orthogonal configuration, unusual configurations are expected in low-symmetry transition-metal dichalcogenide semimetals, which could add flexibility to the electrical injection and detection of pure spin currents. Here, we report the observation of spin-to-charge conversion in MoTe2 flakes, which are stacked in graphene lateral spin valves. We detect two distinct contributions arising from the conversion of two different spin orientations. In addition to the conventional conversion where the spin polarization is orthogonal to the charge current, we also detect a conversion where the spin polarization and the charge current are parallel. Both contributions, which could arise either from bulk spin Hall effect or surface Edelstein effect, show large efficiencies comparable to the best spin Hall metals and topological insulators. Our finding enables the simultaneous conversion of spin currents with any in-plane spin polarization in one single experimental configuration.

The Route to Supercurrent Transparent Ferromagnetic Barriers in Superconducting Matrix.

A ferromagnetic barrier thinner than the coherence length in high-temperature superconductors is realized in the multilayers of YBa2Cu3O7-δ and La0.67Ca0.33MnO3. We used epitaxial growth of YBCO on ⟨110⟩ SrTiO3 substrates by pulsed laser deposition to prepare thin superconducting films with copper oxide planes oriented at an angle to the substrate surface. Subsequent deposition of LCMO and finally a second YBCO layer produces a superconductor/ferromagnet/superconductor trilayer containing an ultrathin ferromagnetic barrier with sophisticated geometry at which the long axis of coherence length ovoid of YBCO is pointing across the LCMO ferromagnetic layer. A detailed characterization of this structure is achieved using high-resolution electron microscopy.