Search

Electrical transport in non-centrosymmetric materials departs from the well-established phenomenological Ohm's law. Instead of a linear relation between current and electric field, a non-linear conductivity emerges along specific crystallographic directions. This non-linear transport is fundamentally related to the lack of spatial inversion symmetry. However, the experimental implications of an inversion symmetry operation on the non-linear conductivity remain to be explored. Here, we report on a large, non-linear conductivity in chiral Tellurium. By measuring samples with opposite handedness, we demonstrate that the non-linear transport is odd under spatial inversion. Furthermore, by applying an electrostatic gate, we modulate the non-linear output by a factor of 300, reaching the highest reported value excluding engineered heterostructures. Our results establish chiral Te as an ideal compound not just to study the fundamental interplay between crystal structure, symmetry operations and non-linear transport, but also to develop wireless rectifiers and energy-harvesting chiral devices., Comment: 7 pages, 4 figures, Supplemental Material

The development of spin-orbitronic devices, such as magneto-electric spin-orbit logic devices, calls for materials with a high resistivity and a high spin-charge interconversion efficiency. One of the most promising candidates in this regard is sputtered Bi$_x$Se$_{1-x}$. Although there are several techniques to quantify spin-charge interconversion, to date reported values for sputtered Bi$_x$Se$_{1-x}$ have often been overestimated due to spurious effects related to local currents combined with a lack of understanding of the effect of the interfaces and the use of approximations for unknown parameters, such as the spin diffusion length. In the present study, non-local spin valves are used to inject pure spin currents into Bi$_x$Se$_{1-x}$, allowing us to directly obtain its spin diffusion length as well as its spin Hall angle, from 10 K up to 300 K. These values, which are more accurate than those previously reported in sputtered Bi$_x$Se$_{1-x}$, evidence that the efficiency of this material is not exceptional. Indeed, the figure of merit for spin-charge interconversion, given by the product of these two parameters, is slightly under 1 nm. Our work demonstrates the importance of considering all material parameters and interfaces when quantifying the spin transport properties of materials with strong spin-orbit coupling., Comment: 12 pages, 4 figures, 1 table, and Supplemental Material

The field of quantum technology has been rapidly expanding in the past decades, yielding numerous applications as quantum information, quantum communication and quantum cybersecurity. The central building block for these applications is a quantum emitter (QE), a controllable source of single photons or photon pairs. Semiconductor QEs such as perovskite nanocrystals (PNCs) and semiconductor quantum dots (QDs) have been demonstrated to be a promising material for pure single-photon emission, and their hybrids with plasmonic nanocavities may serve as sources of photon pairs. Here we have designed a system in which individual quantum emitters and their ensembles can be traced before, during, and after the interaction with the external plasmonic metasurface in controllable way. Upon coupling the external plasmonic metasurface to the array of QEs, the individual QEs switch from single-photon to photon-pair emission mode. Remarkably, this method does not affect the chemical structure and composition of the QEs, allowing them to return to their initial state after decoupling from the plasmonic metasurface. By employing this approach, we have successfully demonstrated the reversible switching of the ensemble of individual semiconductor QEs between single-photon and photon pair emission modes. This significantly broadens the potential applications of semiconductor QEs in quantum technologies.

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 BiFeO$_3$ 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 BiFeO$_3$, 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 BiFeO$_3$. This study constitutes the building block for magnetoelectric spin-orbit logic, opening a new avenue for low-power beyond-CMOS technologies., Comment: 16 pages, 5 figures and Supplementary Information

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 tailor magnetic materials is molecular functionalization, which leads to hybrid interface states with peculiar magnetic properties, called spinterfaces. However, spinterface effects have not yet been explored on layered magnetic materials. Here, we demonstrate the emergence of spinterface effects at the interface between flakes of the prototypical layered magnetic metal Fe3GeTe2 and thin films of paramagnetic Co-phthalocyanine. Magnetotransport measurements show that the molecular layer induces a magnetic exchange bias in Fe3GeTe2, indicating that the unpaired spins in Co-phthalocyanine develop antiferromagnetic ordering by proximity and pin the magnetization reversal of Fe3GeTe2. The effect is strongest for a Fe3GeTe2 thickness of 20 nm, for which the exchange bias field reaches -840 Oe and is measurable up to approximately 110 K. This value compares very favorably with previous exchange bias fields reported for Fe3GeTe2 in all-inorganic van der Waals heterostructures, demonstrating the potential of molecular functionalization to tailor the magnetism of van der Waals layered materials.

Topological materials are of high interest due to the promise to obtain low power and fast memory devices based on efficient spin-orbit torque switching or spin-orbit magnetic state read-out. In particular, sputtered polycrystalline Bi$_x$Se$_{1-x}$ is one of the materials with more potential for this purpose since it is relatively easy to fabricate and has been reported to have a very high spin Hall angle. We study the spin-to-charge conversion in Bi$_x$Se$_{1-x}$ using the spin pumping technique coming from the ferromagnetic resonance in a contiguous permalloy thin film. We put a special emphasis on the interfacial properties of the system. Our results show that the spin Hall angle of Bi$_x$Se$_{1-x}$ has an opposite sign to the one of Pt. The charge current arising from the spin-to-charge conversion is, in contrast, lower than Pt by more than one order of magnitude. We ascribe this to the interdiffusion of Bi$_x$Se$_{1-x}$ and permalloy and the changes in chemical composition produced by this effect, which is an intrinsic characteristic of the system and is not considered in many other studies.

Spin-orbitronic devices can integrate memory and logic by exploiting spin-charge interconversion (SCI), which is optimized by design and materials selection. In these devices, such as the magnetoelectric spin-orbit (MESO) logic, interfaces are crucial elements as they can prohibit or promote spin flow in a device as well as possess spin-orbit coupling resulting in interfacial SCI. Here, we study the origin of SCI in a Py/Cu/W lateral spin valve and quantify its efficiency. An exhaustive characterization of the interface between Cu and W electrodes uncovers the presence of an oxidized layer (WO$_x$). We determine that the SCI occurs at the Cu/WO$_x$ interface with a temperature-independent interfacial spin-loss conductance of $G_{||} \approx$ 20 $\times$ 10$^{13} \Omega^{-1}m^{-2}$ and an interfacial spin-charge conductivity $\sigma_{SC}=-$1610 $\Omega^{-1}cm^{-1}$ at 10 K ($-$830 $\Omega^{-1}cm^{-1}$ at 300 K). This corresponds to an efficiency given by the inverse Edelstein length $\lambda_{IEE}=-$0.76 nm at 10 K ($-$0.4 nm at 300 K), which is remarkably larger than in metal/metal and metal/oxide interfaces and bulk heavy metals. The large SCI efficiency at such an oxidized interface is a promising candidate for the magnetic readout in MESO logic devices., Comment: 11 pages, 3 figures, and Supplemental Material

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 is easily neglected or underestimated. Here, we demonstrate all electrical spin-to-charge conversion in Bi$_x$Se$_{1-x}$ 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., Comment: Main text (18 pages, 3 figures, 2 tables) and supporting information (18 pages)

The Spin Hall magnetoresistance (SMR) emerged as a reference tool to investigate the magnetic properties of materials with an all-electrical set-up. 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 damaged interfaces can yield an important contribution to SMR, questioning a widespread assumption on the role of disorder in such measurements.

Chiral materials are the 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 are excellent electrical transport materials, but have not been explored to enable the electrical control of spin polarization in devices. 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.

Spin-charge interconversion in systems with spin-orbit coupling has provided a new route for the generation and detection of spin currents in functional devices for memory and logic such as spin-orbit torque switching in magnetic memories or magnetic state reading in spin-based logic. Disentangling the bulk (spin Hall effect) from the interfacial (inverse spin galvanic effect) contribution has been a common issue to properly quantify the spin-charge interconversion in these systems, being the case of Au paradigmatic. Here, we obtain a large spin-charge interconversion at a highly conducting Au/Cu interface which is experimentally shown to arise from the inverse spin galvanic effect of the interface and not from the spin Hall effect of bulk Au. We use two parameters independent of the microscopic details to properly quantify the spin-charge interconversion and the spin losses due to the interfacial spin-orbit coupling, providing an adequate benchmarking to compare with any spin-charge interconversion system. The good performance of this metallic interface, not based in Bi, opens the path to the use of much simpler light/heavy metal systems.

Spin Hall magnetoresistance (SMR) refers to a resistance change in a metallic film reflecting the magnetization direction of a magnet attached to the film. The mechanism of this phenomenon is spin exchange between conduction-electron spins and magnetization at the interface. SMR has been used to read out information written in a small magnet and to detect magnetization dynamics, but it has been limited to magnets; magnetic ordered phases or instability of magnetic phase transition has been believed to be indispensable. Here, we report the observation of SMR in a paramagnetic insulator Gd$_{3}$Ga$_{5}$O$_{12}$ (GGG) without spontaneous magnetization combined with a Pt film. The paramagnetic SMR can be attributed to spin-transfer torque acting on localized spins in GGG. We determine the efficiencies of spin torque and spin-flip scattering at the Pt/GGG interface, and demonstrate these quantities can be tuned with external magnetic fields. The results clarify the mechanism of spin-transport at a metal/paramagnetic insulator interface, which gives new insight into the spintronic manipulation of spin states in paramagnetic systems., Comment: 40 pages, 15 figures

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 ($G_s$, $G_r$ and $G_i$), disentangling the contribution of field-like torque ($G_i$), damping-like torque ($G_r$), and spin-flip scattering ($G_s$). An interfacial exchange field of the order of 1 meV acting upon the conduction electrons of Pt can be estimated from $G_i$, which is at least three times larger than $G_r$ below the Curie temperature. Our work provides an easy method to quantify this interfacial spin-splitting field, which play a key role in emerging fields such as superconducting spintronics and caloritronics, and topological quantum computation., Comment: 15 pages, 3 figures, Supporting information included at the end

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 MoTe$_2$ 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., Comment: 14 pages, 4 figures, and Supporting Information

Scattering-type scanning near-field optical microscopy (s-SNOM) allows for nanoscale resolved Infrared (IR) and Terahertz (THz) imaging, and thus has manifold applications ranging from materials to biosciences. However, a quantitatively accurate understanding of image contrast formation at materials boundaries, and thus spatial resolution is a surprisingly unexplored terrain. Here we introduce the write/read head of a commercial hard disk drive (HDD) as a most suitable test sample for fundamental studies, given its well20 defined sharp material boundaries perpendicular to its ultra-smooth surface. We obtainunprecedented and unexpected insights into the s-SNOM image formation process, free of topography-induced artifacts that often mask and artificially modify the pure near-field optical contrast. Across metal-dielectric boundaries, we observe non-point-symmetric line profiles for both IR and THz illumination, which are fully corroborated by numericalsimulations. We explain our findings by a sample-dependent confinement and screening of the near fields at the tip apex, which will be of crucial importance for an accurate understanding and proper interpretation of high-resolution s-SNOM images of nanocomposite materials. We also demonstrate that with ultra-sharp tungsten tips the apparent width (and thus resolution) of sharp material boundaries can be reduced to about 5 nm.

Enhancing magneto-optical effects is crucial for size reduction of key photonic devices based on non-reciprocal propagation of light and to enable active nanophotonics. We disclose a so far unexplored approach that exploits dark plasmons to produce an unprecedented amplification of magneto-optical activity. We designed and fabricated non-concentric magnetoplasmonic-disk/plasmonic-ring-resonator nanocavities supporting multipolar dark modes. The broken geometrical symmetry of the design enables coupling with free-space light and hybridization of dark modes of the ring nanoresonator with the dipolar localized plasmon resonance of the magnetoplasmonic disk. Such hybridization generates a multipolar resonance that amplifies the magneto-optical response of the nanocavity by ~1-order of magnitude with respect to the maximum enhancement achievable by localized plasmons in bare magnetoplasmonic nanoantennas. This large amplification results from the peculiar and enhanced electrodynamic response of the nanocavity, yielding an intense magnetically-activated radiant magneto-optical dipole driven by the low-radiant multipolar resonance. The concept proposed is general and, therefore, our results open a new path that can revitalize research and applications of magnetoplasmonics to active nanophotonics and flat optics., Comment: Supplementary Information included

The Raman response of new structures grown after filling SWCNTs with ferrocene and transformation at moderate high temperatures is demonstrated to be very strong, even stronger than the response from the tubes. Transmission electron microscopy demonstrates that the new objects are flat and exhibit a structure similar to short fragments of nanoribbons. The growth process is controlled by two different activation energies for low and high transformation temperatures, respectively. Immediately after filling Raman pattern from a precursor molecule are detected. Two different types of nanoribbons were identified by selecting special laser energies for the Raman excitation. These ribbons have the signature of quaterrylene and terrylene, respectively., Comment: 6 pages

Spin-to-charge current interconversions are widely exploited for the generation and detection of pure spin currents and are key ingredients for future spintronic devices including spin-orbit torques and spin-orbit logic circuits. In case of the spin Hall effect, different mechanisms contribute to the phenomenon and determining the leading contribution is peremptory for achieving the largest conversion efficiencies. Here, we experimentally demonstrate the dominance of the intrinsic mechanism of the spin Hall effect in highly-resistive Ta. We obtain an intrinsic spin Hall conductivity for $\beta$-Ta of -820$\pm$120 ($\hbar$/e) $\Omega^{-1}cm^{-1}$ from spin absorption experiments in a large set of lateral spin valve devices. The predominance of the intrinsic mechanism in Ta allows us to linearly enhance the spin Hall angle by tuning the resistivity of Ta, reaching up to -35$\pm$3%, the largest reported value for a pure metal., Comment: 9 pages and 4 figures + Supplemental Material (2 pages, 3 figures)

A next-generation memory device utilizing a three-dimensional nanowire system requires the reliable control of domain wall motion. In this letter, domain walls are studied in cylindrical nanowires consisting of alternating segments of cobalt and nickel. The material interfaces acting as domain wall pinning sites, are utilized in combination with current pulses, to control the position of the domain wall, which is monitored using magnetoresistance measurements. Magnetic force microscopy results further confirm the occurrence of current assisted domain wall depinning. Data bits are therefore shifted along the nanowire by sequentially pinning and depinning a domain wall between successive interfaces, a requirement necessary for race-track type memory devices. We demonstrate that the direction, amplitude and duration of the applied current pulses determine the propagation of the domain wall across pinning sites. These results demonstrate a multi-bit cylindrical nanowire device, utilizing current assisted data manipulation. The prospect of sequential pinning and depinning in these nanowires allows the bit density to increase by several Tbs, depending on the number of segments within these nanowires.

The use of magnetic insulators is attracting a lot of interest due to a rich variety of spin-dependent phenomena with potential applications to spintronic devices. Here we report ultra-thin yttrium iron garnet (YIG) / gadolinium iron garnet (GdIG) insulating bilayers on gadolinium iron garnet (GGG). From spin Hall magnetoresistance (SMR) and X-ray magnetic circular dichroism measurements, we show that the YIG and GdIG magnetically couple antiparallel even in moderate in-plane magnetic fields. The results demonstrate an all-insulating equivalent of a synthetic antiferromagnet in a garnet-based thin film heterostructure and could open new venues for insulators in magnetic devices. As an example, we demonstrate a memory element with orthogonal magnetization switching that can be read by SMR., Comment: 12 pages, 5 figures, Supplemental Material (3 pages)

Van der Waals (vdW) materials exhibit intriguing structural, electronic and photonic properties. Electron Energy Loss Spectroscopy (EELS) within Scanning Transmission Electron Microscope (STEM) allows for nanoscale mapping of such properties. However, typical STEM-EELS detection is limited to energy losses in the eV range, which are too large for probing important low-energy excitation such as phonons or mid-IR plasmons. Here we adapt a conventional STEM-EELS system to probe energy loss down to 100 meV, and apply it to map phononic states in h-BN, a representative van der Waals (vdW) material. The h-BN EELS spectra, surprisingly, depend on the h-BN thickness and the distance of the electron beam to h-BN flake edges. To explain this observation, we developed a classical response theory describing the interaction of fast electrons with (anisotropic) slabs of vdW materials. Theoretical and numerical calculations perfectly match the experimental h-BN spectra, and reveal that the electron loss is dominated by the excitation of hyperbolic phonon polaritons, and not of bulk phonons as often reported. Thus, STEM-EELS offers the possibility to probe low-energy polaritons in vdW materials, with our theory being of fundamental importance for interpreting future experiments.

Graphene has been predicted to develop a magnetic moment by proximity effect when placed on a ferromagnetic film, a promise that could open exciting possibilities in the fields of spintronics and magnetic data recording. In this work, we study in detail the interplay between the magnetoresistance of graphene and the magnetization of an underlying ferromagnetic insulating film. A clear correlation between both magnitudes is observed but we find, through a careful modelling of the magnetization and the weak localization measurements, that such correspondence can be explained by the effects of the magnetic stray fields arising from the ferromagnetic insulator. Our results emphasize the complexity arising at the interface between magnetic and two-dimensional materials.

We study by high-resolution transmission electron microscopy the structural response of bilayer graphene to electron irradiation with energies below the knock-on damage threshold of graphene. We observe that one type of divacancy, which we refer to as the butterfly defect, is formed for radiation energies and doses for which no vacancies are formed in clean monolayer graphene. By using first principles calculations based on density-functional theory, we analyze two possible causes related with the presence of a second layer that could explain the observed phenomenon: an increase of the defect stability or a catalytic effect during its creation. For the former, the obtained formation energies of the defect in monolayer and bilayer systems show that the change in stability is negligible. For the latter, ab initio molecular dynamics simulations indicate that the threshold energy for direct expulsion does not decrease in bilayer graphene as compared with monolayer graphene, and we demonstrate the possibility of creating divacancies through catalyzed intermediate states below this threshold energy. The estimated cross section agrees with what is observed experimentally. Therefore, we show the possibility of a catalytic pathway for creating vacancies under electron radiation below the expulsion threshold energy., Comment: 12 pages, 8 figures

We report on the detection and charge distribution analysis for nitrogen substitutional dopants in single layer graphene membranes by aberration-corrected high-resolution transmission electron microscopy (HRTEM). Further, we show that the ionicity of single-layer hexagonal boron nitride can be confirmed from direct images. For the first time, we demonstrate by a combination of HRTEM experiments and first-principles electronic structure calculations that adjustments to the atomic potentials due to chemical bonding can be discerned in HRTEM images. Our experiments open a way to discern electronic configurations in point defects or other non-periodic arrangements or nanoscale objects that can not be analyzed in an electron or x-ray diffraction experiment., Comment: Article and supplementary information, v2 one more figure