Nonvolatile Electric Control of Antiferromagnet CrSBr.

van der Waals magnets are emerging as a promising material platform for electric field control of magnetism, offering a pathway toward the elimination of external magnetic fields from spintronic devices. A further step is the integration of such magnets with electrical gating components that would enable nonvolatile control of magnetic states. However, this approach remains unexplored for antiferromagnets, despite their growing significance in spintronics. Here, we demonstrate nonvolatile electric field control of magnetoelectric characteristics in van der Waals antiferromagnet CrSBr. We integrate a CrSBr channel in a flash-memory architecture featuring charge trapping graphene multilayers. The electrical gate operation triggers a nonvolatile 200% change in the antiferromagnetic state of CrSBr resistance by manipulating electron accumulation/depletion. Moreover, the nonvolatile gate modulates the metamagnetic transition field of CrSBr and the magnitude of magnetoresistance. Our findings highlight the potential of manipulating magnetic properties of antiferromagnetic semiconductors in a nonvolatile way.

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.

Molecular Approach to Engineer Two-Dimensional Devices for CMOS and beyond-CMOS Applications.

Two-dimensional materials (2DMs) have attracted tremendous research interest over the last two decades. Their unique optical, electronic, thermal, and mechanical properties make 2DMs key building blocks for the fabrication of novel complementary metal-oxide-semiconductor (CMOS) and beyond-CMOS devices. Major advances in device functionality and performance have been made by the covalent or noncovalent functionalization of 2DMs with molecules: while the molecular coating of metal electrodes and dielectrics allows for more efficient charge injection and transport through the 2DMs, the combination of dynamic molecular systems, capable to respond to external stimuli, with 2DMs makes it possible to generate hybrid systems possessing new properties by realizing stimuli-responsive functional devices and thereby enabling functional diversification in More-than-Moore technologies. In this review, we first introduce emerging 2DMs, various classes of (macro)molecules, and molecular switches and discuss their relevant properties. We then turn to 2DM/molecule hybrid systems and the various physical and chemical strategies used to synthesize them. Next, we discuss the use of molecules and assemblies thereof to boost the performance of 2D transistors for CMOS applications and to impart diverse functionalities in beyond-CMOS devices. Finally, we present the challenges, opportunities, and long-term perspectives in this technologically promising field.

Gate-Tunable Spin Hall Effect in an All-Light-Element Heterostructure: Graphene with Copper Oxide.

Graphene is a light material for long-distance spin transport due to its low spin-orbit coupling, which at the same time is the main drawback for exhibiting a sizable spin Hall effect. Decoration by light atoms has been predicted to enhance the spin Hall angle in graphene while retaining a long spin diffusion length. Here, we combine a light metal oxide (oxidized Cu) with graphene to induce the spin Hall effect. Its efficiency, given by the product of the spin Hall angle and the spin diffusion length, can be tuned with the Fermi level position, exhibiting a maximum (1.8 ± 0.6 nm at 100 K) around the charge neutrality point. This all-light-element heterostructure shows a larger efficiency than conventional spin Hall materials. The gate-tunable spin Hall effect is observed up to room temperature. Our experimental demonstration provides an efficient spin-to-charge conversion system free from heavy metals and compatible with large-scale fabrication.

Dual-Band Coupling of Phonon and Surface Plasmon Polaritons with Vibrational and Electronic Excitations in Molecules.

Strong coupling (SC) between light and matter excitations bears intriguing potential for manipulating material properties. Typically, SC has been achieved between mid-infrared (mid-IR) light and molecular vibrations or between visible light and excitons. However, simultaneously achieving SC in both frequency bands remains unexplored. Here, we introduce polaritonic nanoresonators (formed by h-BN layers on Al ribbons) hosting surface plasmon polaritons (SPPs) at visible frequencies and phonon polaritons (PhPs) at mid-IR frequencies, which simultaneously couple to excitons and molecular vibrations in an adjacent layer of CoPc molecules, respectively. Employing near-field optical nanoscopy, we demonstrate the colocalization of near fields at both visible and mid-IR frequencies. Far-field transmission spectroscopy of the nanoresonator structure covered with a layer of CoPc molecules shows clear mode splittings in both frequency ranges, revealing simultaneous SPP-exciton and PhP-vibron coupling. Dual-band SC may offer potential for manipulating coupling between exciton and molecular vibration in future optoelectronics, nanophotonics, and quantum information applications.

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.

Tailoring Photoluminescence by Strain-Engineering in Layered Perovskite Flakes.

Strain is an effective strategy to modulate the optoelectronic properties of 2D materials, but it has been almost unexplored in layered hybrid organic-inorganic metal halide perovskites (HOIPs) due to their complex band structure and mechanical properties. Here, we investigate the temperature-dependent microphotoluminescence (PL) of 2D (C6H5CH2CH2NH3)2Cs3Pb4Br13 HOIP subject to biaxial strain induced by a SiO2 ring platform on which flakes are placed by viscoelastic stamping. At 80 K, we found that a strain of <1% can change the PL emission from a single peak (unstrained) to three well-resolved peaks. Supported by micro-Raman spectroscopy, we show that the thermomechanically generated strain modulates the bandgap due to changes in the octahedral tilting and lattice expansion. Mechanical simulations demonstrate the coexistence of tensile and compressive strain along the flake. The observed PL peaks add an interesting feature to the rich phenomenology of photoluminescence in 2D HOIPs, which can be exploited in tailored sensing and optoelectronic devices.

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.

Coherent Phononics of van der Waals Layers on Nanogratings.

Strain engineering can be used to control the physical properties of two-dimensional van der Waals (2D-vdW) crystals. Coherent phonons, which carry dynamical strain, could push strain engineering to control classical and quantum phenomena in the unexplored picosecond temporal and nanometer spatial regimes. This intriguing approach requires the use of coherent GHz and sub-THz 2D phonons. Here, we report on nanostructures that combine nanometer thick vdW layers and nanogratings. Using an ultrafast pump-probe technique, we generate and detect in-plane coherent phonons with frequency up to 40 GHz and hybrid flexural phonons with frequency up to 10 GHz. The latter arises from the periodic modulation of the elastic coupling of the vdW layer at the grooves and ridges of the nanograting. This creates a new type of a tailorable 2D periodic phononic nanoobject, a flexural phononic crystal, offering exciting prospects for the ultrafast manipulation of states in 2D materials in emerging quantum technologies.

Tailoring Superconductivity in Large-Area Single-Layer NbSe2 via Self-Assembled Molecular Adlayers.

Two-dimensional transition metal dichalcogenides (TMDs) represent an ideal testbench for the search of materials by design, because their optoelectronic properties can be manipulated through surface engineering and molecular functionalization. However, the impact of molecules on intrinsic physical properties of TMDs, such as superconductivity, remains largely unexplored. In this work, the critical temperature (TC) of large-area NbSe2 monolayers is manipulated, employing ultrathin molecular adlayers. Spectroscopic evidence indicates that aligned molecular dipoles within the self-assembled layers act as a fixed gate terminal, collectively generating a macroscopic electrostatic field on NbSe2. This results in an ∼55% increase and a 70% decrease in TC depending on the electric field polarity, which is controlled via molecular selection. The reported functionalization, which improves the air stability of NbSe2, is efficient, practical, up-scalable, and suited to functionalize large-area TMDs. Our results indicate the potential of hybrid 2D materials as a novel platform for tunable superconductivity.

Electrical Control of Valley-Zeeman Spin-Orbit-Coupling-Induced Spin Precession at Room Temperature.

The ultimate goal of spintronics is achieving electrically controlled coherent manipulation of the electron spin at room temperature to enable devices such as spin field-effect transistors. With conventional materials, coherent spin precession has been observed in the ballistic regime and at low temperatures only. However, the strong spin anisotropy and the valley character of the electronic states in 2D materials provide unique control knobs to manipulate spin precession. Here, by manipulating the anisotropic spin-orbit coupling in bilayer graphene by the proximity effect to WSe_{2}, we achieve coherent spin precession in the absence of an external magnetic field, even in the diffusive regime. Remarkably, the sign of the precessing spin polarization can be tuned by a back gate voltage and by a drift current. Our realization of a spin field-effect transistor at room temperature is a cornerstone for the implementation of energy efficient spin-based logic.

Spin Hall Effect in Bilayer Graphene Combined with an Insulator up to Room Temperature.

Spin-orbit coupling in graphene can be enhanced by chemical functionalization, adatom decoration, or proximity with a van der Waals material. As it is expected that such enhancement gives rise to a sizable spin Hall effect, a spin-to-charge current conversion phenomenon of technological relevance, it has sparked wide research interest. However, it has only been measured in graphene/transition-metal dichalcogenide van der Waals heterostructures with limited scalability. Here, we experimentally demonstrate the spin Hall effect up to room temperature in graphene combined with a nonmagnetic insulator, an evaporated bismuth oxide layer. The measured spin Hall effect arises most likely from an extrinsic mechanism. With a large spin-to-charge conversion efficiency, scalability, and ease of integration to electronic devices, we show a promising material heterostructure suitable for spin-based device applications.

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.

Room-Temperature Spin Hall Effect in Graphene/MoS2 van der Waals Heterostructures.

Graphene is an excellent material for long-distance spin transport but allows little spin manipulation. Transition-metal dichalcogenides imprint their strong spin-orbit coupling into graphene via the proximity effect, and it has been predicted that efficient spin-to-charge conversion due to spin Hall and Rashba-Edelstein effects could be achieved. Here, by combining Hall probes with ferromagnetic electrodes, we unambiguously demonstrate experimentally the spin Hall effect in graphene induced by MoS2 proximity and for varying temperatures up to room temperature. The fact that spin transport and the spin Hall effect occur in different parts of the same material gives rise to a hitherto unreported efficiency for the spin-to-charge voltage output. Additionally, for a single graphene/MoS2 heterostructure-based device, we evidence a superimposed spin-to-charge current conversion that can be indistinguishably associated with either the proximity-induced Rashba-Edelstein effect in graphene or the spin Hall effect in MoS2. By a comparison of our results to theoretical calculations, the latter scenario is found to be the most plausible one. Our findings pave the way toward the combination of spin information transport and spin-to-charge conversion in two-dimensional materials, opening exciting opportunities in a variety of future spintronic applications.

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.

Activating the molecular spinterface.

The miniaturization trend in the semiconductor industry has led to the understanding that interfacial properties are crucial for device behaviour. Spintronics has not been alien to this trend, and phenomena such as preferential spin tunnelling, the spin-to-charge conversion due to the Rashba-Edelstein effect and the spin-momentum locking at the surface of topological insulators have arisen mainly from emergent interfacial properties, rather than the bulk of the constituent materials. In this Perspective we explore inorganic/molecular interfaces by looking closely at both sides of the interface. We describe recent developments and discuss the interface as an ideal platform for creating new spin effects. Finally, we outline possible technologies that can be generated thanks to the unique active tunability of molecular spinterfaces.

Fullerene-Based Materials as Hole-Transporting/Electron-Blocking Layers: Applications in Perovskite Solar Cells.

Here we report for the first time an efficient fullerene-based compound, FU7, able to act as hole-transporting material (HTM) and electron blocking contact. It has been applied on perovskite solar cells (PSCs), obtaining 0.81 times the efficiency of PSCs with the standard HTM, spiro-OMeTAD, with the additional advantage that this performance is reached without any additive introduced in the HTM layer. Moreover, as a proof of concept, we have described for the first time efficient PSCs in which both selective contacts are fullerene derivatives, to obtain unprecedented "fullerene sandwich" PSCs.

Tunable Sign Change of Spin Hall Magnetoresistance in Pt/NiO/YIG Structures.

Spin Hall magnetoresistance (SMR) has been investigated in Pt/NiO/YIG structures in a wide range of temperature and NiO thickness. The SMR shows a negative sign below a temperature that increases with the NiO thickness. This is contrary to a conventional SMR theory picture applied to the Pt/YIG bilayer, which always predicts a positive SMR. The negative SMR is found to persist even when NiO blocks the spin transmission between Pt and YIG, indicating it is governed by the spin current response of the NiO layer. We explain the negative SMR by the NiO "spin flop" coupled with YIG, which can be overridden at higher temperature by positive SMR contribution from YIG. This highlights the role of magnetic structure in antiferromagnets for transport of pure spin current in multilayers.

Hanle Magnetoresistance in Thin Metal Films with Strong Spin-Orbit Coupling.

We report measurements of a new type of magnetoresistance in Pt and Ta thin films. The spin accumulation created at the surfaces of the film by the spin Hall effect decreases in a magnetic field because of the Hanle effect, resulting in an increase of the electrical resistance as predicted by Dyakonov [Phys. Rev. Lett. 99, 126601 (2007)]. The angular dependence of this magnetoresistance resembles the recently discovered spin Hall magnetoresistance in Pt/Y(3)Fe(5)O(12) bilayers, although the presence of a ferromagnetic insulator is not required. We show that this Hanle magnetoresistance is an alternative simple way to quantitatively study the coupling between charge and spin currents in metals with strong spin-orbit coupling.

Modulation of spin accumulation by nanoscale confinement using electromigration in a metallic lateral spin valve.

We study spin transport in lateral spin valves with constricted channels. Using electromigration, we modulate the spin accumulation by continuously varying the width of the non-magnetic (NM) channel at a single location. By fitting the non-local spin signal data as a function of the NM channel resistance, we extract all the relevant parameters regarding spin transport from a single device. Simulations show that constricting the channel blocks the diffusion of the accumulated spins rather than causing spin flipping. This result could be used to improve the design of future spintronic devices devoted to information processing.