Controlling the helicity of light by electrical magnetization switching.

Controlling the intensity of emitted light and charge current is the basis of transferring and processing information1. By contrast, robust information storage and magnetic random-access memories are implemented using the spin of the carrier and the associated magnetization in ferromagnets2. The missing link between the respective disciplines of photonics, electronics and spintronics is to modulate the circular polarization of the emitted light, rather than its intensity, by electrically controlled magnetization. Here we demonstrate that this missing link is established at room temperature and zero applied magnetic field in light-emitting diodes2-7, through the transfer of angular momentum between photons, electrons and ferromagnets. With spin-orbit torque8-11, a charge current generates also a spin current to electrically switch the magnetization. This switching determines the spin orientation of injected carriers into semiconductors, in which the transfer of angular momentum from the electron spin to photon controls the circular polarization of the emitted light2. The spin-photon conversion with the nonvolatile control of magnetization opens paths to seamlessly integrate information transfer, processing and storage. Our results provide substantial advances towards electrically controlled ultrafast modulation of circular polarization and spin injection with magnetization dynamics for the next-generation information and communication technology12, including space-light data transfer. The same operating principle in scaled-down structures or using two-dimensional materials will enable transformative opportunities for quantum information processing with spin-controlled single-photon sources, as well as for implementing spin-dependent time-resolved spectroscopies.

Large and tunable magnetoresistance in van der Waals ferromagnet/semiconductor junctions.

Magnetic tunnel junctions (MTJs) with conventional bulk ferromagnets separated by a nonmagnetic insulating layer are key building blocks in spintronics for magnetic sensors and memory. A radically different approach of using atomically-thin van der Waals (vdW) materials in MTJs is expected to boost their figure of merit, the tunneling magnetoresistance (TMR), while relaxing the lattice-matching requirements from the epitaxial growth and supporting high-quality integration of dissimilar materials with atomically-sharp interfaces. We report TMR up to 192% at 10 K in all-vdW Fe3GeTe2/GaSe/Fe3GeTe2 MTJs. Remarkably, instead of the usual insulating spacer, this large TMR is realized with a vdW semiconductor GaSe. Integration of semiconductors into the MTJs offers energy-band-tunability, bias dependence, magnetic proximity effects, and spin-dependent optical-selection rules. We demonstrate that not only the magnitude of the TMR is tuned by the semiconductor thickness but also the TMR sign can be reversed by varying the bias voltages, enabling modulation of highly spin-polarized carriers in vdW semiconductors.

Epitaxial Kagome Thin Films as a Platform for Topological Flat Bands.

Systems with flat bands are ideal for studying strongly correlated electronic states and related phenomena. Among them, kagome-structured metals such as CoSn have been recognized as promising candidates due to the proximity between the flat bands and the Fermi level. A key next step will be to realize epitaxial kagome thin films with flat bands to enable tuning of the flat bands across the Fermi level via electrostatic gating or strain. Here, we report the band structures of epitaxial CoSn thin films grown directly on the insulating substrates. Flat bands are observed by using synchrotron-based angle-resolved photoemission spectroscopy (ARPES). The band structure is consistent with density functional theory (DFT) calculations, and the transport properties are quantitatively explained by the band structure and semiclassical transport theory. Our work paves the way to realize flat band-induced phenomena through fine-tuning of flat bands in kagome materials.

Vacancy-engineered nodal-line semimetals.

Symmetry-enforced nodal-line semimetals are immune to perturbations that preserve the underlying symmetries. This intrinsic robustness enables investigations of fundamental phenomena and applications utilizing diverse materials design techniques. The drawback of symmetry-enforced nodal-line semimetals is that the crossings of energy bands are constrained to symmetry-invariant momenta in the Brillouin zone. On the other end are accidental nodal-line semimetals whose band crossings, not being enforced by symmetry, are easily destroyed by perturbations. Some accidental nodal-line semimetals have, however, the advantage that their band crossings can occur in generic locations in the Brillouin zone, and thus can be repositioned to tailor material properties. We show that lattice engineering with periodic distributions of vacancies yields a hybrid type of nodal-line semimetals which possess symmetry-enforced nodal lines and accidental nodal lines, with the latter endowed with an enhanced robustness to perturbations. Both types of nodal lines are explained by a symmetry analysis of an effective model which captures the relevant characteristics of the proposed materials, and are verified by first-principles calculations of vacancy-engineered borophene polymorphs. Our findings offer an alternative path to relying on complicated compounds to design robust nodal-line semimetals; one can instead remove atoms from a common monoatomic material.

Fusion of Majorana bound states with mini-gate control in two-dimensional systems.

A hallmark of topological superconductivity is the non-Abelian statistics of Majorana bound states (MBS), its chargeless zero-energy emergent quasiparticles. The resulting fractionalization of a single electron, stored nonlocally as a two spatially-separated MBS, provides a powerful platform for implementing fault-tolerant topological quantum computing. However, despite intensive efforts, experimental support for MBS remains indirect and does not probe their non-Abelian statistics. Here we propose how to overcome this obstacle in mini-gate controlled planar Josephson junctions (JJs) and demonstrate non-Abelian statistics through MBS fusion, detected by charge sensing using a quantum point contact, based on dynamical simulations. The feasibility of preparing, manipulating, and fusing MBS in two-dimensional (2D) systems is supported in our experiments which demonstrate the gate control of topological transition and superconducting properties with five mini gates in InAs/Al-based JJs. While we focus on this well-established platform, where the topological superconductivity was already experimentally detected, our proposal to identify elusive non-Abelian statistics motivates also further MBS studies in other gate-controlled 2D systems.

Evidence for anisotropic spin-triplet Andreev reflection at the 2D van der Waals ferromagnet/superconductor interface.

Fundamental symmetry breaking and relativistic spin-orbit coupling give rise to fascinating phenomena in quantum materials. Of particular interest are the interfaces between ferromagnets and common s-wave superconductors, where the emergent spin-orbit fields support elusive spin-triplet superconductivity, crucial for superconducting spintronics and topologically-protected Majorana bound states. Here, we report the observation of large magnetoresistances at the interface between a quasi-two-dimensional van der Waals ferromagnet Fe0.29TaS2 and a conventional s-wave superconductor NbN, which provides the possible experimental evidence for the spin-triplet Andreev reflection and induced spin-triplet superconductivity at ferromagnet/superconductor interface arising from Rashba spin-orbit coupling. The temperature, voltage, and interfacial barrier dependences of the magnetoresistance further support the induced spin-triplet superconductivity and spin-triplet Andreev reflection. This discovery, together with the impressive advances in two-dimensional van der Waals ferromagnets, opens an important opportunity to design and probe superconducting interfaces with exotic properties.

Large Tunneling Magnetoresistance in van der Waals Ferromagnet/Semiconductor Heterojunctions.

2D layered chalcogenide semiconductors have been proposed as a promising class of materials for low-dimensional electronic, optoelectronic, and spintronic devices. Here, all-2D van der Waals vertical spin-valve devices, that combine the 2D layered semiconductor InSe as a spacer with the 2D layered ferromagnetic metal Fe3 GeTe2 as spin injection and detection electrodes, are reported. Two distinct transport behaviors are observed: tunneling and metallic, which are assigned to the formation of a pinhole-free tunnel barrier at the Fe3 GeTe2 /InSe interface and pinholes in the InSe spacer layer, respectively. For the tunneling device, a large magnetoresistance (MR) of 41% is obtained under an applied bias current of 0.1 µA at 10 K, which is about three times larger than that of the metallic device. Moreover, the tunneling device exhibits a lower operating bias current but a more sensitive bias current dependence than the metallic device. The MR and spin polarization of both the metallic and tunneling devices decrease with increasing temperature, which can be fitted well by Bloch's law. These findings reveal the critical role of pinholes in the MR of all-2D van der Waals ferromagnet/semiconductor heterojunction devices.

Quantum Spin-Valley Hall Kink States: From Concept to Materials Design.

We propose a general and tunable platform to realize high-density arrays of quantum spin-valley Hall kink (QSVHK) states with spin-valley-momentum locking based on a two-dimensional hexagonal topological insulator. Through the analysis of Berry curvature and topological charge, the QSVHK states are found to be topologically protected by the valley-inversion and time-reversal symmetries. Remarkably, the conductance of QSVHK states remains quantized against both nonmagnetic short- and long-range and magnetic long-range disorder, verified by the Green-function calculations. Based on first-principles results and our fabricated samples, we show that QSVHK states, protected with a gap up to 287 meV, can be realized in bismuthene by alloy engineering, surface functionalization, or electric field, supporting nonvolatile applications of spin-valley filters, valves, and waveguides even at room temperature.

Water-Dispersible CsPbBr3 Perovskite Nanocrystals with Ultra-Stability and its Application in Electrochemical CO2 Reduction.

Thanks to the excellent optoelectronic properties, lead halide perovskites (LHPs) have been widely employed in high-performance optoelectronic devices such as solar cells and light-emitting diodes. However, overcoming their poor stability against water has been one of the biggest challenges for most applications. Herein, we report a novel hot-injection method in a Pb-poor environment combined with a well-designed purification process to synthesize water-dispersible CsPbBr3 nanocrystals (NCs). The as-prepared NCs sustain their superior photoluminescence (91% quantum yield in water) for more than 200 days in an aqueous environment, which is attributed to a passivation effect induced by excess CsBr salts. Thanks to the ultra-stability of these LHP NCs, for the first time, we report a new application of LHP NCs, in which they are applied to electrocatalysis of CO2 reduction reaction. Noticeably, they show significant electrocatalytic activity (faradaic yield: 32% for CH4, 40% for CO) and operation stability (> 350 h).

Synthesis, Magnetic Properties, and Electronic Structure of Magnetic Topological Insulator MnBi2Se4.

The intrinsic magnetic topological insulators MnBi2Te4 and MnBi2Se4 support novel topological states related to symmetry breaking by magnetic order. Unlike MnBi2Te4, the study of MnBi2Se4 has been inhibited by the lack of bulk crystals, as the van der Waals (vdW) crystal is not the thermodynamic equilibrium phase. Here, we report the layer-by-layer synthesis of vdW MnBi2Se4 crystals using nonequilibrium molecular beam epitaxy. Atomic-resolution scanning transmission electron microscopy and scanning tunneling microscopy identify a well-ordered vdW crystal with septuple-layer base units. The magnetic properties agree with the predicted layered antiferromagnetic ordering but disagree with its predicted out-of-plane orientation. Instead, our samples exhibit an easy-plane anisotropy, which is explained by including dipole-dipole interactions. Angle-resolved photoemission spectroscopy reveals the gapless Dirac-like surface state, which demonstrates that MnBi2Se4 is a topological insulator above the magnetic-ordering temperature. These studies show that MnBi2Se4 is a promising candidate for exploring rich topological phases of layered antiferromagnetic topological insulators.

Phase Signature of Topological Transition in Josephson Junctions.

Topological superconductivity holds promise for fault-tolerant quantum computing. While planar Josephson junctions are attractive candidates to realize this exotic state, direct phase measurements as the fingerprint of the topological transition are missing. By embedding two gate-tunable Al/InAs Josephson junctions in a loop geometry, we measure a π jump in the junction phase with an increasing in-plane magnetic field B_{∥}. This jump is accompanied by a minimum of the critical current, indicating a closing and reopening of the superconducting gap, strongly anisotropic in B_{∥}. Our theory confirms that these signatures of a topological transition are compatible with the emergence of Majorana bound states.

Optically Probing Tunable Band Topology in Atomic Monolayers.

In many atomically thin materials, their optical absorption is dominated by excitonic transitions. It was recently found that optical selection rules in these materials are influenced by the band topology near the valleys. We propose that gate-controlled band ordering in a single atomic monolayer, through changes in the valley winding number and excitonic transitions, can be probed in helicity-resolved absorption and photoluminescence. This predicted tunable band topology is confirmed by combining an effective Hamiltonian and a Bethe-Salpeter equation for an accurate description of excitons, with first-principles calculations suggesting its realization in Sb-based monolayers.

Localized Excitons in NbSe2-MoSe2 Heterostructures.

Neutral and charged excitons (trions) in atomically thin materials offer important capabilities for photonics, from ultrafast photodetectors to highly efficient light-emitting diodes and lasers. Recent studies of van der Waals (vdW) heterostructures comprised of dissimilar monolayer materials have uncovered a wealth of optical phenomena that are predominantly governed by interlayer interactions. Here, we examine the optical properties in NbSe2-MoSe2 vdW heterostructures, which provide an important model system to study metal-semiconductor interfaces, a common element in optoelectronics. Through low-temperature photoluminescence (PL) microscopy, we discover a sharp emission feature, L1, that is localized at the NbSe2-capped regions of MoSe2. L1 is observed at energies below the commonly studied MoSe2 excitons and trions and exhibits temperature- and power-dependent PL consistent with exciton localization in a confining potential. This PL feature is robust, observed in a variety of samples fabricated with different stacking geometries and cleaning procedures. Using first-principles calculations, we reveal that the confinement potential required for exciton localization naturally arises from the in-plane band bending due to the changes in the electron affinity between pristine MoSe2 and NbSe2-MoSe2 heterostructure. We discuss the implications of our studies for atomically thin optoelectronics devices with atomically sharp interfaces and tunable electronic structures.

Phase Control of Majorana Bound States in a Topological X Junction.

Topological superconductivity supports exotic Majorana bound states (MBS) which are chargeless zero-energy emergent quasiparticles. With their non-Abelian exchange statistics and fractionalization of a single electron stored nonlocally as a spatially separated MBS, they are particularly suitable for implementing fault-tolerant topological quantum computing. While realizing MBS has focused on one-dimensional systems, the onset of topological superconductivity requires delicate parameter tuning and geometric constraints pose significant challenges for their control and demonstration of non-Abelian statistics. To overcome these challenges, building on recent experiments in planar Josephson junctions (JJs), we propose a MBS platform of X-shaped JJs. This versatile implementation reveals how external flux control of the superconducting phase difference can generate and manipulate multiple MBS pairs to probe non-Abelian statistics. The underlying topological superconductivity exists over a large parameter space, consistent with materials used in our fabrication of such X junctions, as an important step towards scalable topological quantum computing.

Ultrafast spin-lasers.

Lasers have both ubiquitous applications and roles as model systems in which non-equilibrium and cooperative phenomena can be elucidated1. The introduction of novel concepts in laser operation thus has potential to lead to both new applications and fundamental insights2. Spintronics3, in which both the spin and the charge of the electron are used, has led to the development of spin-lasers, in which charge-carrier spin and photon spin are exploited. Here we show experimentally that the coupling between carrier spin and light polarization in common semiconductor lasers can enable room-temperature modulation frequencies above 200 gigahertz, exceeding by nearly an order of magnitude the best conventional semiconductor lasers. Surprisingly, this ultrafast operation of the resultant spin-laser relies on a short carrier spin relaxation time and a large anisotropy of the refractive index, both of which are commonly viewed as detrimental in spintronics3 and conventional lasers4. Our results overcome the key speed limitations of conventional directly modulated lasers and offer a prospect for the next generation of low-energy ultrafast optical communication.

Dynamical screening in monolayer transition-metal dichalcogenides and its manifestations in the exciton spectrum.

Monolayer transition-metal dichalcogenides (ML-TMDs) offer exciting opportunities to test the manifestations of many-body interactions through changes in the charge density. The two-dimensional character and reduced screening in ML-TMDs lead to the formation of neutral and charged excitons with binding energies orders of magnitude larger than those in conventional bulk semiconductors. Tuning the charge density by a gate voltage leads to profound changes in the optical spectra of excitons in ML-TMDs. On the one hand, the increased screening at large charge densities should result in a blueshift of the exciton spectral lines due to reduction in the binding energy. On the other hand, exchange and correlation effects that shrink the band-gap energy at elevated charge densities (band-gap renormalization) should result in a redshift of the exciton spectral lines. While these competing effects can be captured through various approximations that model long-wavelength charge excitations in the Bethe-Salpeter equation, we show that a novel coupling between excitons and shortwave charge excitations is essential to resolve several experimental puzzles. Unlike ubiquitous and well-studied plasmons, driven by collective oscillations of the background charge density in the long-wavelength limit, we discuss the emergence of shortwave plasmons that originate from the short-range Coulomb interaction through which electrons transition between the [Formula: see text] and [Formula: see text] valleys. The shortwave plasmons have a finite energy-gap because of the removal of spin-degeneracy in both the valence- and conduction-band valleys (a consequence of breaking of inversion symmetry in combination with strong spin-orbit coupling in ML-TMDs). We study the coupling between the shortwave plasmons and the neutral exciton through the self-energy of the latter. We then elucidate how this coupling as well as the spin ordering in the conduction band give rise to an experimentally observed optical sideband in electron-doped W-based MLs, conspicuously absent in electron-doped Mo-based MLs or any hole-doped ML-TMDs. While the focus of this review is on the optical manifestations of many-body effects in ML-TMDs, a systematic description of the dynamical screening and its various approximations allow one to revisit other phenomena, such as nonequilibrium transport or superconducting pairing, where the use of the Bethe-Salpeter equation or the emergence of shortwave plasmons can play an important role.

Spin inversion in graphene spin valves by gate-tunable magnetic proximity effect at one-dimensional contacts.

Graphene has remarkable opportunities for spintronics due to its high mobility and long spin diffusion length, especially when encapsulated in hexagonal boron nitride (h-BN). Here, we demonstrate gate-tunable spin transport in such encapsulated graphene-based spin valves with one-dimensional (1D) ferromagnetic edge contacts. An electrostatic backgate tunes the Fermi level of graphene to probe different energy levels of the spin-polarized density of states (DOS) of the 1D ferromagnetic contact, which interact through a magnetic proximity effect (MPE) that induces ferromagnetism in graphene. In contrast to conventional spin valves, where switching between high- and low-resistance configuration requires magnetization reversal by an applied magnetic field or a high-density spin-polarized current, we provide an alternative path with the gate-controlled spin inversion in graphene.

Magnetic Proximity Effects in Transition-Metal Dichalcogenides: Converting Excitons.

The two-dimensional character and reduced screening in monolayer transition-metal dichalcogenides (TMDs) lead to the ubiquitous formation of robust excitons with binding energies orders of magnitude larger than in bulk semiconductors. Focusing on neutral excitons, bound electron-hole pairs that dominate the optical response in TMDs, it is shown that they can provide fingerprints for magnetic proximity effects in magnetic heterostructures. These proximity effects cannot be described by the widely used single-particle description but instead reveal the possibility of a conversion between optically inactive and active excitons by rotating the magnetization of the magnetic substrate. With recent breakthroughs in fabricating Mo- and W-based magnetic TMD heterostructures, this emergent optical response can be directly tested experimentally.